MINOR AND TRACE ELEMENTS - OSTI.GOV

XA0054839

MINOR AND TRACE ELEMENTS

G.V. lyengar and L Tandon

3 1 / 2 5

FOREWORD

As part of a Co-ordinated Research Project (CRP) on Comparative International Studies ofOsteoporosis Using Isotope Techniques, the International Atomic Energy Agency (IAEA) hasrecently supported some studies of trace elements in human bones. In connection with this work,the need became apparent for an up-to-date literature review of minor and trace elements inhuman bones. The authors of this report were commissioned with the task of doing this, and werealso requested to extend their review to cover human teeth. Their report is reproduced in thisform mainly to make it available to the participants in the abovementioned CRP. However, it ishoped that the report will also be of interest to a wider audience. The IAEA would like to expressits thanks to the authors. Any comments on the report would be welcome; they should be sentdirectly to the authors* with a copy to the IAEA's Section of Nutritional and Health-RelatedEnvironmental Studies.

Addresses for correspondence:

G.V. IyengarBiomineral Sciences International Inc.6202 Maiden LaneBethesda,MD 20817USA

L.Tandon505 Oppenheimer Drive #503Los Alamos, NM 87544USA

Section of Nutritional and Health-Related Environmental StudiesInternational Atomic Energy AgencyP.O. Box 100A-1400 ViennaAUSTRIA

TABLE OF CONTENTS

1. Introduction 1

2. Basis for data collection 1

3. Bone 23.1 Bones in the human body 23.2 Characteristics of bone 23.3 Methods for sampling bone 43.4 Methods for processing bone 4

4. Tooth 54.1 The human teeth 54.2 Characteristics of tooth 54.3 Methods for sampling tooth 54.4 Methods for processing tooth 6

5. Analysis 65.1 Analytical methods 65.2 Reference materials for bone and teeth 75.3 Preparation of bone and teeth for measurement 7

6. Elemental composition of bones 86.1 Major and minor elements 86.2 Trace elements 9

7. Elemental composition of teeth 127.1 Major and minor elements 137.2 Trace elements 13

8. Discussion 168.1 Limitations of the data compiled 168.2 Major and minor elements in bones and teeth 168.3 Trace elements in bones and teeth 16

9. Concluding remarks 18

10. References 19

ANNEXES (Data compilation)

Table 1: Range of Mean Values for Major, Minor and Trace Elements in Human Bones 23

Table 2: Range of Mean Values for Major, Minor and Trace Elements in Human Teeth 25Table 3: Major, Minor and Trace Elements in Human Bones 31Table 4: Major, Minor and Trace Elements in Human Teeth 69Figures 88References (for compiled data) 93

1. INTRODUCTION

Bone is a major compartment of the skeletal system. It is a living, dynamic structure which provides asupporting and protective framework for the body. Bone provides a reservoir of calcium and phosphate andalso has functions in magnesium metabolism. The core contains marrow, which serves as a reservoir ofnutrients and produces several types of blood cells. Bone consists of 35 % mineral salts (chiefly calcium andphosphorus), 20 % organic matrix (of which 95 % is collagen), and 45 % water. About 99 % of body calciumis found in bone. Besides numerous organic constituents, bone is also a major pool for some trace elements.Trace elements such as F, Sr, Pb and U are predominantly found in bone, and are generally termed as boneseekers.

Bone is an example of a biological sample that presents numerous difficulties in obtaining a specimen forchemical analysis. This problem is acute when investigations are to be conducted to determine total skeletalcontent of a given analyte. First of all, the basic process of sampling bone can be a very difficult task. Withhumans, this problem is compounded due to medico-legal implications. Not withstanding these obstacles,the question of which particular bone qualifies to be a representative sample of the skeleton as a whole (ifat all) is a debatable point. Even if some assumptions are made to answer this question, the sub-compartments of a bone sample, namely cortical, trabecular and the marrow and their relative proportion andsignificance in relation to bone as an organ, present intricate situations in making definitive decisions. Choiceof multiple types of bones is of course the best solution but it is beset with logistical aspects of procuringmany bone specimens depending upon the scope of the investigation.

Therefore, it is not surprising that reliable chemical composition data, particularly for minor and traceelements, are scarce. This is also substantiated by the fact that there are only a couple of certified bonereference materials available for validating analytical methods. However, a survey of the scientific literatureshows that some analytical work has been expended to establish the elemental composition profile of bone.The usefulness of such analytical information depends upon whether or not analytical quality control wasexercised at least to some degree so that an evaluation of the results can be undertaken to identify referencevalues.

Arguments, similar to that of bone can also be extended to human teeth, with the exception that some of themedico-legal implications are less restrictive than those surrounding human bone sampling.

The purpose of this report is to screen literature information on the elemental composition data for humanbone and teeth and to identify reference range of values where data permit such conclusions. This report willalso include a concise assessment of the sampling practices in use, and measurement techniques that areapplicable for elemental analysis of bones and teeth.

2. BASIS FOR DATA COLLECTION

There have been a few sources, [1-4] which have attempted to shed some light on the activities taking placein understanding the elemental composition profile of bones. Of these, the publication of The Reference Manby the International Commission on Radiological Protection (ICRP) [1] marks an important milestone in theelemental composition of the human body. This excellent source documents analytical results generatedduring the years 1950-1970 (mainly) for human tissues including bone, carried out in the mainly in the 60s.However, limitations arising from inadequacies of methodologies practiced at the time ICRP-23 waspublished were recognized by the analytical community and efforts continued to generate accurate data toimprove existing information as well as to cover fresh grounds for those elements for which data were notavailable. An account of part of that analytical improvements has been summarized in a compilation [5] byexpanding the scope of elemental coverage. Since then, further improvements have taken place in analytical

approaches, especially with the availability of certified reference materials (CRM) for analytical qualitycontrol and therefore, generally speaking the status of trace element analysis in tissue samples is at a stagewhere reasonably reliable results are being generated. Moreover, many investigations are designed to reflectinterdisciplinary perspectives [6] and this has further enhanced the overall quality and validity of the sampledspecimen. Finally, sustained application of analytical techniques such as the Inductively Coupled PlasmaMass Spectrometry (ICP-MS) has spurred the field of biological trace element research. Hence a freshevaluation of the literature results is useful to scrutinize the situation and explore the possibility of evaluatingreference values.

3. BONE

3.1 Bones in the human body

The human skeletal system and associated major groups of bones are shown in Figure 1. Temporal, vertebra,ribs, sternum, humerus, ilium, ulna, femur and tibia are examples of sources used to obtain autopsy or biopsysamples. Tibia is a readily accessible bone. Similarly, rib samples are sought at autopsy. Iliac crest isusually the sampling site of choice for histologic examination of trabecular bone.

3.2 Characteristics of bone

Bone is composed of osseous tissue, a tissue made hard by the deposition of inorganic substances in a processknown as calcification. Other segments of this system are teeth, bone marrow, periosteum and all cartilageof the body. Periarticular tissue, also referred to as connective tissue is situated at joints such as hip and kneeand is firmly attached to the bone structure. It is difficult to separate it from the bones during dissection andtherefore, sometimes becomes part of the skeletal weight and partly contributes to the variations observedin skeletal weights. Bone as a tissue represents an organic matrix the bulk of which is made up of the proteincollagen. The inorganic matter consists mainly of deposits of calcium phosphate. On the other hand, boneas an organ comprises of red and yellow marrow, cartilage periosteum, blood and the bone tissue.

Based on the hardness, porosity and the content of soft tissue present in them bone tissue is commonlydivided into two compartments: compact (cortical) bone and trabecular (spongy and porous) bone. However,not all bones can be strictly classified as compact or trabecular since some types are intermediate in porosityand difficult to classify.

The compact bone is the hard dense part surrounding the outer walls of all bones, and it is predominant inthe shafts of the long bones. Bone forming cells called the osteoblasts, synthesize the organic matrix(osteoid), tissue which undergoes mineralization. The trabecular bone is a spongy formation seen at theinterior of flat bones and at the ends of long bones. It is highly porous (being soft and consisting mainly ofbone marrow). It is also referred to as osseous tissue of the trabeculae, and if the matter also includes the softtissue part then it is referred to as spongiosa.

Some investigators use the terminologies such as cancellous (spongy) bone and petrous (hard or the compact)bones.

In adults, typically 75-85 % of the total bone mass is considered to be compact bone and the rest trabecularbone [7,8]. After the skeleton has matured there is a continual net loss in trabecular bone mass, amountingto 25-45 % of the peak trabecular mass in normal human beings [9]. In the femur, there is considerably morebone loss with advancing age in trabecular than in cortical bone [10].

A typical long bone (femur, humerus) is a thick-walled, hollow, cylindrical shaft (the diaphysis) of compactbone. The central marrow cavity is the medulla. The ends of the shaft, mainly spongy bone covered by a thincortex of compact bone, are called epiphysis. When actual growth is taking place, the epiphysis and thediaphysis are separated by columns of spongy bone (the metaphysis). Most bones are covered by theperiosteum, a specialized connective tissue layer which can, if necessary, contribute to the formation of newbone.

The density of the skeleton is about 1.3 g/cc, and that of the dry mineralized collagenous bone matrix is closeto 2.3 g/cc [11]. The mean density of vertebral cortical and trabecular bones has been reported to be 1.99and 1.92 g/cc, respectively [12]. Densities reported for bones from Caucasian subjects aged 79 are as follow:fresh compact bone (from shafts of tibiae and femora) 1.85 g/cc, where as for fresh spongiosa (trabecularbone with marrow taken from thoracic and lumbar vertebrae and the calcaneus) was 1.08 g/cc [13]. Theseauthors have also reported variations in densities between several subsamples taken from the same area ofone bone. For example, the density of spongiosa (thoracic vertebrae) was found to be 0.8 to 1.4 g/cc, whiledensities of cortical bones (mid-schaft of the tibia) ranged from 1.5 to 2 g/cc.

The inorganic fraction is made of crystals forming hexagonal plates which are deposited in a regular way onand parallel to the axis of the collagen fibers. Bone crystals consist chiefly of hydroxyapatite, but they alsocontain carbonate, citrate and small amounts of sodium, magnesium, potassium, chloride, fluoride, and anumber of trace elements. The crystals are surrounded by a hydration shell which allows free exchange ofions between extracellular fluid and the interior of crystals. Ions at the interior of the crystals have a slowturnover rate (some ions known as bone-seekers such as uranium, plutonium, lead, strontium and radium canbe easily incorporated into the crystals).

The calcified mass of adult bone has three types of surface: a surface on which nothing seems to happenunder normal physiological conditions (about 90 % of bone surface); a surface on which bone is being formed(controlled by osteoblasts, single nuclear cells); and a surface at which bone is being resorbed (boneresorption is controlled by multinuclear gain cells called osteoclast). Bone formation and bone resorptionoccur continuously and simultaneously throughout life, although the rates change with age and vary indifferent parts of the skeleton.

3.2 Representative bone samples

Homogeneity even within a particular type of bone samples is a much debated topic and it may be safely saidthat there are many diverse opinions. This is understandable because of the variations in proportions of theconstituent compartments in a given bone segment, and the dynamics of bone growth.

The criterion for defining a particular bone sample as representative specimen mainly depends upon its usageand the associated logistics in obtaining the desired section of the bone. For example, in dealing with bonefracture cases, iliac crest will be biopsied for clinical studies since it can be done safely and easily. However,these biopsies serve as a proxy for those bones that suffer from fractures (e.g. osteoporosis), although iliaccrest itself does not directly suffer from fractures. The argument here is that some one that has osteoporosisat one site is likely to have it generalized and that the iliac crest is probably representative. There is evidencethat among various bones, iliac crest presents the best scenario of homogeneity [14]. On the other hand, boneis readily available in large amounts from subjects that fracture their hips and also from subjects undergoinghip replacement (e.g. arthritis). These situations offer other sampling possibilities for acquiring both normaland pathologic bone specimens.

The autopsy situation although beset with medico-legal barriers, when these barriers are overcome, offers thepossibility of collecting rib, long bones, vertebrae etc, and have been the sources of bone samples. In manyautopsy studies aimed at collecting skeletal data for radiological purposes, these sample have been frequently

analyzed. Some times only a single type of specimen has been analyzed, and in some cases a combinationof bones has been investigated.

In summary, with the exception of in vivo possibilities for assessment of total body Ca (and a few otherelements) for diagnostic and other purposes (where facilities are available), despite severe limitations facedin obtaining biopsy samples from living subjects, this practice remains inevitable. Samples from autopsycases, in spite of the fact that they too suffer from different type of limitations, provide the only practicalpossibility for undertaking comprehensive skeletal elemental concentration profile studies. Where possible,collection of multiple types of samples, analysis, and averaging the results for each skeletal segment wouldenhance the reliability of total skeletal content data.

3.3 Methods for sampling bone

Large quantities of bone samples are obtained at autopsy while limited quantities of biopsy specimens(especially as a part of a clinical procedure) are obtained by surgical intervention.

Biopsy sampling from living subjects require the usual sterile requirements and limitations on what type ofgadgets can be used. Usually, a 8 mm diameter stainless steel trephine is used to obtain bone biopsy samples.The recovered quantity of bone permits separation of cortical and trabecular portions of bone by processingunder clean bench conditions. Practical steps involved in such operations are presented in Figure 2 based onthe procedure developed by Inskip et al [15]. Although this particular example is from a study designed tobiopsy bones in monkeys, the technical aspects provide useful information for processing human samples.

Sampling at autopsy on the other hand, would permit use of conventional clean stainless steel equipment forremoval of a section of bone from the body. After removal, samples are packaged in plastic bags and shippedunder cool conditions (e.g. dry ice) to carry out the remaining part of the sampling operations that can beperformed in the laboratory.

3.4 Methods for processing bone

Removal of connective tissues, soft tissues, fat and fibers is required. In some cases marrow part has to beseparated. All these operations require considerable efforts and clean working conditions if the samples areintended for trace analysis.

Primary fragmentation of a chunk of bone can be accomplished by cooling the bone in liquid nitrogen andimpacting it with a suitable implement. However, to avoid the risk of contamination and to provide a safecontainment for the sample during the handling process, the sample should be enclosed in a Teflon bag andthen cooled. Wedging the cooled bone between two plastic slabs (e.g. perspex blocks) and then impactingit with a stainless steel hammer would minimize such acontamination risk. This procedure yields small segments of samples and facilitates removal of marrow andother constituents, as well as partitioning the sample into subsections.

Distilled water, ether, acetone, chloroform, methanol, hydrogen peroxide and glacial acetic acid have beenused separately or as mixtures have for defatting and cleaning. For cutting operations depending upon thepurpose of the investigation, tools made of stainless steel and tungsten carbide can be used. It may even bepossible to use tools made of quartz and titanium for finer operations or to remove soft parts of the bone thusminimizing exposure to hard metals. These tools can be cleaned with 1 % EDTA solution, followed byultrasonic cleaning with demineralized water an methanol (10 %).

The processed samples should be preferably freeze-dried and stored under cool conditions until taken up forthe measurement phase (see section 5.3).

4. TOOTH

4.1 The human teeth

The human adult has 32 permanent teeth. In each of the dental arcade there are two incisors, one canine, twopremolar, and three molars.

In children, teeth are classified as deciduous or permanent. Deciduous teeth are formed during childhood andthey are 20 in number: Incisors (central=4, lateral=4), canines =4, and molars (lst=4, 2nd=4). In additionthere are 12 permanent: premolars=8 and 3rd molars=4.

The primary function of teeth is to mince food into small particles to pass through the esophagus.

4.2 Characteristics of tooth

The teeth consists of crowns that project above the gum, and single or multiple roots. Incisors have one root,lower and upper molars two and three roots, respectively.

The hard components of teeth are dentine, enamel, cementum (specific gravity 3.0, 2.14 and 2.03,respectively), with dentine being the bulk component surrounding the chamber that contains the pulp.Dentine has no blood vessels or nerve fibers. Those that line the inner surface of dentine, known asodontoblast, maintain the dentine deposits. The water content of dentine and cementum is about 10 % on aweight basis. Dentine also contains some firmly bound water. The pulp, being a soft tissue contains morewater.

Enamel, which is the outer surface of tooth, is formed prior to eruption by epithelial cells called ameloblast.This is the hardest part in the body. Enamel is hydroxyapatite crystals embedded in fibers of keratin. Oncethe process of enamel formation is completed, no new enamel can be added. The water content of enamel isabout 3 %.

The main inorganic constituents of both enamel and dentine are Ca, P, Mg and CO* Almost the entire weightof enamel (dry basis) is inorganic matrix, while that of dry dentine is 80 %.

Cementum, a bony substance is secreted by the periodontal membrane which lines the tooth alveolus (socket).Collagen fibers originating from the jaw bone pass through the periodontal membrane, making their way intocementum, and thus hold the tooth in place.

The pulp, which fills the tooth, consists of connective tissues, nerves, blood vessels and lymphatics. The pulpis a soft tissue in composition and therefore has a higher water content than other compartments [16].

4.3 Methods for sampling tooth

A schematic diagram showing the components of tooth is shown in Figure 3. The sections includes wholetooth, tooth crown (enamel and dentine) and tooth roots (dentine).

Tooth as a whole entity is a heterogeneous matrix with two solid phases which represent different densitiesand also vary in their ability to concentrate trace elements. Therefore, sampling presents rather basicproblems, and makes analysis of whole tooth less meaningful. The degree of variability of trace elementdistribution is further affected by increased sorption from decidual teeth and amalgam fillings (whereapplicable) in teeth from the adults.

Deciduous teeth are obtained from dental clinics or schools or by approaching the parents directly.Occasionally, collection of healthy permanent tooth from living subjects is possible when tooth is extractedfor orthodontal reasons. Hence sampling at autopsy is the only means of obtaining a complete set of samplesthat satisfy statistical design of a particular study. On the other hand, dental clinics are the best sources forpathologic specimens. Since the analysis of whole tooth is not meaningful, processing tooth samples furtherto extract the desired compartments is unavoidable and makes the analytical task rather tedious. The crownof tooth (enamel + dentine) is relatively easy to sample, but the relative proportions of the two tissues varyfrom specimen to specimen and the integrity of the specimen is compromised. Added to this, segments suchas enamel are in such small proportions in a tooth matrix, sample contamination becomes a critical factor.Dentine presents special problems of contamination because of its porosity.

Hence the major problem with tooth is in the sample preparation step.

4.4 Methods for processing tooth

Tooth can be analyzed as a whole sample, or in sections: the sections are surface enamel, bulk enamel, bulkdentine circumpulpal dentine and cementum (enamel-dentine junction). Alternately, the whole tooth, toothcrown (enamel + dentine) and tooth roots (dentine) can also be analyzed. The sample treatment andprocessing steps differ depending upon the aim of the investigation. If the study is designed to investigateonly the healthy teeth, those with fillings or caries should be discarded.

Removal of residual traces of blood, adhering soft tissues if any, and surface contamination will be required.Soaking in hydrogen peroxide, hypochlorite solution, acid wash and even brushing and scraping will facilitateremoval of the residues. A detergent or acetone wash will accomplish removal of grease and fats. Mildscraping or brushing with appropriate tools and rinsing with high purity water is adequate if the teeth havenot developed stains. Several procedures used in this connection have been reviewed [17,18].

Sectioning of teeth is required when whole tooth is not analyzed. Various cutting techniques have been usedfor isolating pulp, enamel and dentine: These include use of a diamond dental saw, dental burr drill, chippingand chiseling [17]. After the precleaning operations with distilled water and mild solvents, the crown (enamel+ dentine) may be separated using the diamond saw. Further, enamel and dentine can also be separated,weighed and taken for further treatment such as dry or wet ashing.

Importantly, after the tooth is cleaned and being prepared for sectioning, the entire operation has to be carriedout under clean conditions. The degree of difficulty posed by different sections during sample preparationis variable. Small quantities of samples obtainable from surface enamel make this part more prone toextraneous contamination. Analysis of bulk enamel, because of its abundance and low porositycharacteristics can be expected to yield reliable results. Dentine on the other hand is a more porous fraction(hence easily contaminated) but it is regarded as a good indicator of lead exposure because of its growthcharacteristics [17].

The processed samples should be preferably freeze-dried and stored under cool conditions until taken up forthe measurement phase (see section 5.3).

5. ANALYSIS

5.1 Analytical methods

A survey of the literature reveals that practically every available analytical technique has been applied todetermine one or the other element in bones and teeth. The methods used are: atomic absorption spectroscopy

(AAS), atomic emission spectroscopy (AES), anodic stripping voltametiy (ASV), mass spectrometiy (MS),X-ray methods particularly proton induced X-ray emission (PIXE) [19] and finally, nuclear activationtechniques. All these techniques have been used in different modes depending upon the quantity of thesample available and elements sought. A review by Zwanziger [20] summarizes the applicability of a varietyof methods for the analysis of bone. In a Canadian effort, a method based on AAS applicable to samples ofa few mg has been demonstrated to be very effective [21].

Similarly, A review by Fergusson and Purchase [17] summarizes the applicability of a variety of methodsfor the analysis of tooth, with special reference to determination of lead.

Both destructive and non-destructive methods of analysis will be required to cover elemental analysis of alarge number of minor and trace elements. Sample processing being a difficult operation for bone and toothsamples, non-destructive techniques such as neutron activation analysis (NAA) and X-ray based techniquessuch as X-ray fluorescence (XRF) and PIXE should be preferred. These techniques are suited for thedetermination of several elements in bone and tooth matrices.

Besides these in-vitro methods, for elements such as Ca in bone, in vivo approaches have also been utilized.

5.2. Reference materials for bone and teeth

There are only a few reference materials that are useful for quality control requirements of hard tissueanalysis. The animal bone CRM (IAEA H-5) issued by the International Atomic Energy Agency (IAEA) iscurrently out of stock. The bone ash (NIST SRM 1400) and bone meal (NIST SRM 1486) issued by theNational Institute of Standards and Technology are presently available. For tooth matrix, not even a singlecertified or recognized control material is presently available.5.3 Preparation of bone and teeth for measurement

If the analysis is desired for whole bone and tooth, a few randomly selected small pieces of a particular typeof bone or a tooth sample can be pulverized using the brittle fracture technique [22]. This procedure, whichderives the benefit of making the samples brittle under liquid nitrogen cooling helps to pulverize thebone/tooth sample. The next treatment depends upon the method of analysis (destructive or non-destructive).

Obviously, the non destructive mode of analysis possible by techniques such as the NAA, PIXE, promptgamma NAA and X-ray-Fluorescence is very attractive since it minimizes the work at the measurement stageof the analysis. It offers the possibility to investigate the variability of a given element on a population basisas large number of samples can be analyzed. Hence, in cases where these methods are applicable and areaccessible, it is definitely of advantage to use them.

Much has been discussed in the literature about the presence of organic matter in bones as a source ofinterference during the measurement process and the need for removal of this fraction prior to analysis.However, if instrumental techniques are used then the samples may have to be merely encapsulated orpelletized and appropriate contamination control procedures have to be followed. On the other hand, ifchemical intervention is required as is the case with some methods, the sample is either digested in high purityacids (wet ashing) or decomposed at low or high temperature depending upon the analyte in question (dryashing). Both of these manipulations have their own short comings and the analyst's insight into theseprocesses play a major role when results are reported.

Edward et al [23] have investigated the problem of dry ashing human and animal bone for a range of ashingtimes and temperatures. They have concluded that fluorine, chlorine, bromine, sodium, potassium and zincwere affected to varying degrees between 400 and 600 degrees C. For example, in the case of zinc it was

shown that rat bone with biologically incorporated radioactive isotope (Zn-65) lost zinc after 6 hours ofashing and continued to lose up to 12 hours (i.e. even after the organic material had been removed). The losswas more pronounced at 500 and 600 °C treatments than at 400°C. Magnesium, calcium, strontium andmanganese were unaffected. Zwanziger [20] has reviewed a number of ashing investigations related to severaladditional elements, and has pointed out in particular the poor reproducibility of results of lead analysis fromashed samples. Use of low temperature ashing aided by oxygen streams and us of Teflon containers forashing have been shown to be safer, should dry ashing is the method of choice. Wet ashing aided bymicrowave oven appears to be the method of choice of many investigators. Dissolution in nitric acid isacceptable for most methods.

Concerning tooth, problems faced with dissolution are similar to that of bone. Teeth sampleshave been extensively analyzed in context of lead and several wet and dry ashing proceduresare applicable if carefully carried out [17].

6. ELEMENTAL CONCENTRATIONS IN BONES

The elemental composition of bone surveyed as part of this review is presented in Table 3. It may beremarked that most publications do not satisfactorily describe the characteristics of the sampled bone as wellas the methods adopted for preparation prior to analysis. Because of this lack of documentation it is verydifficult to attribute whether the often observed differences are real or due simply to unspecified nature ofthe sample. For example, bone samples from aged subjects may have been in the subclinical state ofosteoporosis but are classified as normal bone samples. Or a bone sample may contain small quantities ofresidual marrow and collagen. Under these conditions, analysis for a major element such as Ca would resultin depressed concentration than what is likely to be normal. For the same reason, Fe results may tend to behigh resulting from contributions due to the presence of even traces of red marrow. The reports were checkedfor analytical quality control (AQC) component, in particular to find out whether RM was used for validationof methods. This information is also shown in Table 3. It appears that rib samples are the frequentlyanalyzed part of the skeleton.

6.1 Ca, N, O, P and minor elements

Oxygen; The oxygen component of the bone is reported to be between 30 and 46 %. Some fluctuation dueto changes in moisture content is to be expected. Therefore, the distinction between fresh and dry weightbasis also in not easy to identify.

Nitrogen: The nitrogen component of bone is reported to be between 4.4 to 5 %, with one exception whichreported 12.2 %. The presence of soft tissue (e.g. marrow) and collagen can influence the nitrogenconcentration and may account for high values.

Calcium: As expected, bone has been frequently analyzed for Ca. Besides activation techniques, especiallyNAA for both in vitro and in vivo determination of Ca, AAS and ICP-AES have also been applied. Typicalconcentration ranges reported are: cortical (20 to 22.5 %), trabecular (15.5 to 26 %) and whole bone (17 to26 %). Occasional high and low values are also seen and it is difficult to interpret these results due to smallnumber of samples involved, and methodological implications. No demonstrable link was observed betweenCa concentration and geographical location of the subjects or between different types of bone samples.Similarly, the effects of age,sex, health, diet and metabolism were not readily apparent from the data, probably due to the underlyingstatistical reasons. Large groups of subjects need to be studied and compared. The number of studiesreported from Japan is very impressive. Many groups have used available RMs.

Phosphorus: Results from several countries obtained by different techniques show between 7 and 12.5 %between different types of bones, some based on fresh and some based on dry weight. The results overlapthe stated range both on wet and dry basis and point to the need for establishing a strict protocol for analysisas well as for expressing the results. However, the average in many cases appear to fall within the narrowrange of 10-12.5 % based only on dry weight. Some specific sections of the bone namely concha media andconcha interior have been reported to contain P at concentrations exceeding 30 %.

Chlorine, Potassium, Sodium and Sulfur: Cl concentrations generally vary from 800 to 2700 mg/kg,including the spread from wet to dry basis, with one specific compartment showing as low as 200 mg/kg.Na falls in the range of 3000 to 8000 mg/kg on a dry weight basis. Very few results for K are available forcomments, and there is a wide spread of concentrations reported ranging from about 50 to 6200 (>120 times)mg/kg. Sample characterization and analysis both need to be reviewed for this element before a referencevalue is assigned. For S, concentration of 800 mg/kg reported by one study raises concerns because ofanalytical problems (see section 7).

6.2 Trace elements in bone

Aluminum: ICP-AES has been frequently used by many investigators. Concentration of Al seems to be higherin ribs than in other areas of the skeleton. The results from Japan generally indicate high concentrations ofAl. Al is believed to accumulate in bone with age [24]. Therefore, failure to document the age diminishesthe credibility of the results if used for comparison. The over all range observed between various studiesfalls between 2 to 46 mg/kg. Among specific types of bone, a concentration of 19.5 mg/kg has been reportedfor iliac crest.

Antimony. Instrumental NAA is a good method for determining Sb if the concentration is not at the sub-ppblevel. Very few results are reported for Sb in bone and the available findings suggest the averageconcentration to be in the low ppb range.

Arsenic: As is a difficult element to determine in biological samples, especially in bone. Therefore, it is notsurprising that not many results have been reported for this element. Sample processing, e.g. dry ashing evenat mild conditions can affect recovery. It appears that As is present at about 10 ppb or less.

Barium: Rather wide variations are seen in the results ranging from 1 to 35 mg/kg, when all the investigationsare considered. However, of these a few selected investigations conform to a narrow range of 2.7 to 6 mg/kg,based on dry weight, providing an indication of probable average concentration of Ba in bone.

Boron: Very few results based on systematic studies have been reported for human bone. B is gainingrecognition as a probable essential element for bone metabolism and therefore, there is a need for systematicstudies of B in human bones, especially from different geographic locations and living conditions (e.g.vegetarians vs others). Like As, B is also susceptible to severe losses during processing and requires greatcare in sample preparation stages. The reported results range from 8 mg/kg on a fresh weight for one set ofsamples to 23 mg/kg for another set based on dry weight.

Bromine: Results available from half a dozen investigations suggest a range of 1.4 to 12 mg/kg as probableoverall range (fresh or dry basis) without any clear separation.

Cadmium: AAS has been used by several investigators to determine Cd. A comparison of data spread over6 countries does not reveal any particular trend since analytical problems are largely not resolved. Basedmainly on AAS results, the best estimate for a majority of studies appear to fall in the range of 0.03 to 0.69mg/kg (wet or dry, due to overlapping ranges).

Cobalt: NAA and ICP-AES are well suited for the determination of Co and this is readily reflected in theresults compiled. Based on dry bone, it appears that Co is present in bone at a concentration range of 0.015to 0.13 mg/kg.

Chromium: Cr seems to be present in human bone at the ppm level. Since methods such as NAA permit non-destructive determination, in practice it is possible to minimize contamination. There appears to be areasonable agreement between methods. With the exception of one study from China reporting divergentresults, a concentration of 2.75 to 11 mg/kg appears to be the average range. Most of the samples are derivedfrom ribs and both cortical and cancellous segments of bone have been investigated.

Cesium: NAA and ICP-MS are suitable methods for the determination of Cs. Results from Japan, showO.004 mg/kg by ICP-MS. Italian results based on dry weight indicate a range of 0.03 to 0.06 mg/kg, whilethe Chinese samples show a range of 0.05 to 0.08 mg/kg on ash weight basis.In fact the overall agreement is reasonable (ash weight is close to 50 % of dry weight), but work is neededto define a broad based reference range, since Cs is a radiologically sought element in bone.

Copper: Several analytical techniques have been used to determine Cu in bone. Analysis of bone for Cuinvolves the risk of contamination by reagents when ultra pure chemicals and water are not used duringsample dissolution. Two studies using ICP-AES have reported a concentration exceeding 20 mg/kg (dryweight basis), while those using PIXE have reported between 5-19 mg/kg. Since these investigators did notuse known RMs for AQC, the results seem to be open for discussion. An extensive investigation involvingsamples from USA reported 0.3 to 0.5 mg/kg (wet weight) in a variety of segments such as ribs, skull, tibia,vertebrae from both males and females. The remaining results are spread in the range of 1-5 mg/kg.Therefore, based on the current literature status, although reasonably good number of studies have beendocumented, it is not feasible to recommend a generalized reference value.

Fluorine: There are not many analytical methods (with the exception of ion-selective electrode) that arepractical for the determination of F in biological materials. Nuclear based techniques are applicable only athigh concentrations in specific matrices. This is reflected in very few RMs being certified for F in naturalmatrices. The overall range of concentration reported is 510 to 2100 mg/kg (dry weight). F is known toconcentrate in bone, and this can explain the high values. The concentration of F in cortical (also referredto as compacta) is lower than in trabecular (also known as spongiosa) section. A difference, by a factor of3 has been experimentally demonstrated for a bone sample taken from the distal epiphysis of a femur of askeleton representing preindustrial populations [25]. hi high fluoride areas as in India, bone samples havebeen shown to contain extremely high concentration of F [26]. The F concentration in bone possiblyincreases with age. But this is difficult to ascertain because of the demonstrated inhomogeneity and widevariation in the distribution of F in bone along the length of a bone sample [25].

Iron: AAS, ICP-AES and NAA are most frequently used techniques. Fe concentration depends upon age,sex, diet and metabolism. There is a wide range of values reported for Fe for ribs. Part of the reason maystem from the reasoning presented under section 6. The effect of red (bone) marrow on the concentration ofFe found in bone can be minimized by careful handling of the sample. With the exception of oneinvestigation from Japan, the remaining studies that have reported the results on wet or dry basis, indicatean overall range of 13 to 106 mg/kg. Results based on ash weight reported from China show high values.

Lead: AAS is the most popular method. Pb is one of the extensively studied elements because of the toxicimplications. The risk of contamination during processing and loss during ashing is very high and requiresgood AQC. Concerning distribution of Pb in different sites of a particular type of bone, several differenceshave been observed in a study conducted on a skeleton belonging to preindustrial period [25]. The variationsobserved were, a factor of 2 for femur, 3 for tibia, 2.5 for fibula, 2 for ulna, and 3 for rib. Interestingly, for

10

the hip bone (i.e. iliac crest region) very little variation was observed from point to point, giving an indicationthat iliac crest (e.g. biopsy) maybe a good site for sampling. In Table 3, over 30 sets of results from severalgeographic regions are shown, and a majority of them fall in the range of 2 to 17 mg/kg irrespective of thebasis (wet or dry) used to express the results. Practically every type of bone sample has been investigated.For individual bones, a restricted survey [27] states the following concentration as a general guide foranalytical planning: rib 4-9, vertebra 2-8, femur 7-22, tibia 8-23 and skull 13-24, based on mg/kg dryweight. Bones samples from heavily industrialized and polluted areas generally tend to contain highconcentrations of Pb in them as observed in samples from Poland (up to 70 mg/kg), (Table 3).

Magnesium: AAS, ICP-AES and NAA are applicable techniques. There appears to be not much difficultyin determining Mg in bone since the concentration range is high. A considerable number of studies have beenreported for Mg in bone. The overall range appears to be between 0.17 and 0.37 %, with overlapping rangefor wet and dry weight based results. The samples are mainly from ribs, and include both cortical andtrabecular segments.

Manganese: AAS, ICP-AES and NAA are most frequently used methods. The Mn concentration in boneappears to indicate geographical differences. There is a wide range of results reported by severalinvestigators for various segments of the bone. It is difficult to arrive at a reference value. The overall rangecovers 0.14 to 8 mg/kg, irrespective of the basis used to express the concentrations. Mn is believed to be animportant element in bone metabolism [28]. And several bone developmental effects have been linked tobone growth thus demonstrating the essentiality of Mn in bone metabolism [29].

Mercury: Like As and B, Hg may be easily lost if proper care is not taken during sample processing. Notmany results are reported for this element. Being a nonessential element, the presence of Hg in tissues is anindicator of the exposure to this element through water, food or the conditions representing the environment,and it is difficult to arrive at a generalized reference value. Therefore, the limited results (0.018 to 0.62mg/kg, dry weight basis) listed in Table 3. may be considered to indicate a particular level of exposure.

Molybdenum: There are only a few methods capable of determining Mo in biological materials at the levelMo occurs in these matrices. NAA is a very good method but very few analysts have access to such facilities.For these and other reasons there are only a few Mo results currently available for bone. Much work iswarranted since dietary intake of Mo on a global basis is very different, and may be interesting to study itsimpact on bone metabolism.

Nickel: ICP-AES is the most frequently used method for determination of Ni in bone. A modest number ofanalytical results have been reported for this element. Excluding one high value (9.1 mg/kg) from a Japanesestudy, the remaining values fall in the range of 0.42 to 2.6 mg/kg.

Polonium: Po is a naturally radioactive element and is known as a bone seeker. By counting the radioactivityand making suitable corrections it is possible to assay minute quantities of Po in tissue samples. Results fromtwo studies included in this compilation show Po concentrations well below part per trillion.

Rubidium: Instrumental NAA is particularly suited method for determining Rb in bone. Based on theavailable data, the average concentration may be somewhere in the range of 1 to 9.5 mg/kg. Of the 10investigations included in this compilation, an Australian study that included bone marrow as part of thesample, has reported 25 mg/kg, while one from Russia without adequately defining sample and samplingcharacteristics has found 38 mg/kg.

Strontium: Nuclear analytical methods are very popular. Because of the close relationship with Cametabolism in bone, Sr is an extensively investigated element and results are available from over 20investigations. Not surprisingly, a wide range of results have been reported since bone is a target matrix for

11

Sr accumulation and factors such as intake and age influence the metabolism of Sr in bone. Thus a range of50 to 420 mg/kg (wet or dry basis) seems to represent a plausible average profile. Unfortunately, manypublications do not clearly indicate the geographic origin of the samples within the country Results reportedfrom China and Russia are very high suggesting some environmental and nutritional factors. A clearidentification of the bone area being analyzed, age of the subjects, and sample processing might help explainsome of the extreme values reported in the literature. Sr is a radiologically sought element in bone.

Scandium: Instrumental NAA is particularly suited method for determining Sc in bone, and all the 4 setsof results included in this compilation are obtained by this method. The reported results cover a wide rangefrom 0.001 to 0.19 mg/kg.

Selenium: Instrumental NAA is a good method for determining Se in bone. Based on 6 sets of resultsavailable from this review, 0.1 to 0.6 mg/kg appears to be the target range for reference values. Moreinvestigations are needed for confirmation.

Thorium: ICP-MS and RNAA are the chosen techniques for determining Th in biological matrices. In bone,INAA is also applicable if the concentration is not too low. Because of the limitations of choice of methods,not many investigations have been carried out to establish a broad based data base for Th in biologicalsamples. Of the 2 investigations listed in this compilation, < 0.06 mg/kg has been reported for Japanesesamples, and 0.2 to 0.4 mg/kg (ash basis) for samples from China.

Uranium: Radiochemical methods such as alpha spectrometry are the most sensitive methods for analysisof bones. Recently, ICP-MS has emerged as a powerful technique but the applications are just in thebeginning stage. Results from Australia, USA, Russia, Nepal and China show average concentrations in therange of 0.001 to 0.062 mg/kg on an ash weight basis. Results for Japan are at the low end ranging from0.0003 to 0.0009 mg/kg based on fresh weight of the tissue. Bone is a target organ for U, and is also aradiologically sought element.

Vanadium: Not many investigations are reported. ICP-AES is applicable, so is NAA if radiochemistry isused. The average concentration is probably in the range of 1-4 mg/kg, on a dry weight basis.

Zinc: AAS, ICP-AES, NAA, PIXE and XRF all are suitable for analyzing bone for Zn as reflected bynumerous investigations. NAA is extremely well suited since it involves minimum sample preparation andpurely instrumental determination. Over 25 sets of results for Zn have been scrutinized in this compilation.The average concentration ranges from 25 to 265 mg/kg, with overlapping ranges based on fresh, dry or ashweight. Zn concentrations in bone appear to depend on various factors such as nutrition, metabolism, andenvironment. The results also indicate inhomogeneous distribution of this element within the skeletalsystem. Considering only the U.S. results for rib, skull, tibia and vertebrae from both men and women, therange narrows to 25 - 58 mg/kg, based on fresh weight.

7. ELEMENTAL CONCENTRATIONS IN TEETH

The elemental composition of tooth surveyed as part of this review is presented in Table 4. As in the caseof bone analysis, it should be recognized that most publications do not satisfactorily describe thecharacteristics of the sampled tooth as well as the methods adopted for preparation prior to analysis. Theinvestigation by Cutress [30] studying the composition of the outer layer of dental enamel in samplesobtained from 14 countries is a good example of the logistics involved in planning multi element studies. Theresults for Cu, Ba and S which appear to be extremely high have been traced back to possible methodologicalproblem, in particular to disagreement with analysis of a reference sample. Further, the presence of cariesif unnoticed compromises sample integrity. This is particularly important when teeth samples are sectioned

12

and in the absence of documentation it is very difficult to attribute whether the often observed differences arereal or due simply to unspecified nature of the sampled fraction. For example, tooth samples may have beenexposed to "filler" composites directly or as adjacent specimens. Or a tooth sample may contain smallquantities of residual blood and soft tissue. Under these conditions, analysis for a major element such as Cawould result in depressed concentration than what is likely to be normal. For the same reason. The reportswere checked for AQC, in particular to find out whether RM was used for validating the methods. Thisinformation is also shown in Table 4.

Methods applicable for bone are in principle also applicable to tooth analysis. Therefore, no reference totechniques will be made. Similarly, some of the general comments that can be seen under bone for selectedtrace elements are extendable to tooth, hence the comments under the following sections will be minimized.

7.1 Ca, P and minor elements

Unlike the large number of studies of Ca in bone, teeth appear to have been less widely investigated. Theavailable results suggest the following concentrations: enamel from 31.5 to 37.3 %, dentine 31.5 % andwhole tooth 10-12 % (samples from Polish subjects, appear to be low in concentration of Ca). However,individual investigations for dentine and whole tooth have been carried out less frequently than those forenamel. A link between dietary Ca, environmental factors and Ca content of tooth is not well established.However, more studies would be needed to confirm the relationship. Concerning P, the 5 studies listed inTable 4. show an average range of 16-21 % for enamel and 14 % for dentine. The results for Cl show amixed picture. One set of results for enamel have been reported to be between 1600 to 2800 mg/kg while2 other investigations indicate a range of 8000-9000 mg/kg. In dentine, the reported concentration is closeto 2500 mg/kg, all based on dry weight. The concentration of K in enamel appears to differ widely between190 to 1200 mg/kg, and in whole teeth one set of results are quoted to be just 53 mg/kg. Similarly, Naconcentrations range from 1700 to 1300 mg/kg in enamel, 2000 to 2300 mg/kg in dentine and 1125 to 1193mg/kg in whole tooth. Mg in enamel 745 to 4100 mg/kg, and in dentine around 1000-8000 mg/kg, basedon dry weight. For S, results were available for only enamel showing an average concentration of 300 to1350 mg/kg, with extreme values of 24 and 18780 mg/kg (all based on dry weight), for surface enamel. Thehigh value appears to be due to analytical problem as the control sample has been stated to yield erraticresults [30].

7.2 Trace elements

Aluminum: Results are available from another compilation for 14 countries and 3 other countries are listedin Table 4. The results, available only for enamel cover a wide range between 2 and 343 mg/kg. In somecases the basis used for expressing the results is uncertain and hence no definite comments can be offered forthe presence of Al in teeth. None of the studies mentions the presence of caries in the teeth, and most groupsexercise AQC. AQC check is specially needed in the case of Al since it is a difficult element to determine,and easy to introduce by way of contamination.

Barium: In view of the similarity of Ba with Ca and Sr, several investigations have dealt with these elementsas a group. The overall range is spread between 2 and 22 mg/kg. Even the two studies reporting valuesidentifying the basis (dry) for expression report 6.4 and 22 mg/kg. Hence a definitive statement on Ba intooth enamel is not possible. Available RMs have been used for AQC.

Boron: Results are reported for enamel and the overall range is 1 to 8 mg/kg; Of these 2 investigations havementioned the basis (dry) used, and these values are 4.1 to 5.3 mg/kg.

Bromine: Results are reported for enamel and the overall range is 1 to 4.5 mg/kg; Of these 1 investigationhas mentioned the basis (dry), stating a concentration of 3.1 mg/kg for surface enamel.

13

Cadmium: Results have been reported for several countries. In Poland, Finland and the USA, samples fromseveral geographical regions have been investigated. Available data suggest some dependence of the Cdconcentration with geographical region in a given country. Enamel is the frequently studied fraction and theaverage concentration of Cd in this tissue appears to be in the range of 2 to 9 mg/kg, dry weight. The lowestconcentrations of Cd were measured in dentine samples from Greenland and Denmark (0.086 to 0.097 mg/kg,dry) suggesting environment as a factor. Because of the difficulties in obtaining reliable results for Cd inbiomatrices, the role of AQC has been well recognized in most of the studies. Interestingly, among the resultstabulated in this compilation, studies that adopted strict AQC procedures reported low concentration of Cdin the samples.

Cobalt. The indicative concentrations for dentine and enamel appear to be 0.1 and 0.2 mg/kg, respectively.For whole tooth, the results appear to spread between 5 and 25 mg/kg. Sample characterization being poor,these results must be regarded carefully.

Chromium: Cr in tooth seems to depend upon a number of parameters. The first and the foremost is the AQCaspect. The various fractions show differing Cr concentrations depending upon the origin of the sample.Concentrations as high as 15 to 30, and 20 to 40 mg/kg (dry) have been reported for samples from Australiafor dentine and enamel, respectively, while samples from a number of other countries can be grouped withina narrow range of 0.45 to 3.9 (dry) for both. On the other hand, whole tooth samples from urban and ruralareas of Poland have been reported to contain as much as 42 to 47 mg/kg (dry) of Cr. Hence it is difficultto make any meaningful conclusions based on the available data.

Copper: The compilation includes samples representing many countries, and in several cases either multipleethnic groups or differing geographic regions have been investigated. The results vary from country tocountry and indicate environment as a possible factor for the observed variations. Cu concentration of wholetooth (7 to 10 mg/kg, dry) generally exceeds that of dentine (0.8 to 5 mg/kg, dry?) or enamel (0.2 to 2.75mg/kg, dry). Exceptional concentrations of 10 to 30, and 15-50 mg/kg (dry) have been reported for a set ofenamel and dentine from Australia. Analytically, most investigators are capable of determining Cu withoutmuch difficulty and therefore, the observed variations seem to suggest real variations.

Fluorine: Determination of F in tooth should be scrutinized carefully, since methodologically it is stillconsidered as an unresolved problem. The average concentration of F in enamel appears to fall in the widerange of 55 - 750 mg/kg. Tooth paste is a source of F, and careful documentation concerning dental hygienepractices of individuals is crucial. Therefore, it is difficult to conclude how much of this variation isoriginating from cosmetic sources, and how much is originating from diet and environmental sources, sinceall these are key players in the distribution of F in tissues. Some aspect of has discussed under F in bone(section 6.2).

Iron: There appears to be no clear separation of Fe in dentine, enamel or whole tooth. As seen from Table4, dentine (3 to 30 mg/kg), enamel (15 - 138 mg/kg) and whole tooth (32 to 65 mg/kg), the only tendencyseen relates to the low values seen for dentine. The use of AQC procedures is quite satisfactory. The linkbetween concentration of Fe in tooth and age, diet, section of the tooth analyzed is unclear and needs furtherstudies.

Mercury: Analysis of tooth samples for Hg are susceptible to multiple doubts. Sample preparationprocedures may seriously hamper the status of Hg in the sample, so is the problem of Hg in the laboratoryenvironment. In addition, Hg being part of the filler substance, case history of the sample has to be carefullyscrutinized. The reported results do not indicate any specific tendency as such.

14

Magnesium: AAS and to some extent PIXE have been frequently used to determine Mg in tooth. Mgconcentration in the enamel (specifically from the surface) is generally lower than that found in dentine.There appears to be no specific analytical problem in determining this element in tooth samples.

Manganese: There appears to be some tendency in the distribution of Mn in dentine, enamel and wholetooth. As seen from Table 4, dentine (1-4 mg/kg, except for Australian samples), enamel (0.1 to 2.0 mg/kg,except for Australian samples) and whole tooth (9 to 48 mg/kg). The only general discrepancy seems to behigh in surface enamel as reviewed by Cutress [30]. The link, if any between concentration of Mn in toothand age, diet, and the section of the tooth analyzed, is unclear and needs further studies. There have beensome differences reported for tooth samples from different countries, and it may be due to geographicalconditions. As discussed under Al, contamination problems for Mn are very severe, and extreme care shouldbe exercised duringanalysis.

Molybdenum: Not many results have been reported for Mo. Also the results mostly concern the enamelfraction (0.1 to 2.4 mg/kg, dry), and hence no comments on specific trends can be provided.

Nickel: Nickel resembles Mn and Al in terms of problems faced during analysis, and careful attention tocontamination control is a crucial requirement. Ni in enamel has been identified in the range of 0.4 to 1.2mg/kg, with one value in the high range of 23 mg/kg in surface enamel. In whole tooth the concentrationrange appears to around 5 to 30 mg/kg. More data are required to reliably interpret the Ni concentrations intooth and associated compartments.

Lead: Pb is a frequently investigated element in tooth. Many studies have been reported from several globalregions. The results reported for urban areas are generally higher than those reported for non-urbanenvironments. The following concentrations have been reported: enamel (2 to 150 mg/kg, dry, exceptionstwo sets of samples with 1100 and 1236 mg/kg for surface enamel), dentine (1 to 118 mg/kg, dry), and wholetooth (1 to 48 mg/kg dry, with one set showing 254 to 336 mg/kg on ash weight basis). Pb concentration indentine tends to be high and reflects possible link to age, diet and other environmental factors. There issufficient evidence to account for AQC by most investigators. One reason for this is the underlyingtoxicological importance of the data generated and the care taken during the planning stage of theinvestigation.

Strontium: Results are available from several countries. Very few results were found for whole tooth. Onthe other hand, almost every investigation studied the enamel and dentine fractions, with enamel receivingmore attention in terms of number of studies. Analytically, Sr does not pose serious difficulties, and thereforecomparative information is reliable. The following concentrations have been reported: enamel (82 to 204mg/kg, dry, exception being some individual samples reported to contain concentrations up to 1400 mg/kg,and 7630 mg/kg for surface enamel), dentine (75 to 83 mg/kg, dry, with individual concentrations extendingup to 250 mg/kg). A possible link appears to exist with geographical location but needs further confirmation.

Vanadium: Limited number of studies have addressed the problem of V determination in teeth. The enamelfraction has been analyzed by a couple of investigators and the range of concentrations reported lie between0.003 to 0.02 mg/kg (with one exception reporting 1.2 mg/kg for surface enamel). The results reported forYugoslavia are at the low end of the spectrum, suggesting that the study was conducted carefully with specialattention to AQC. This study reports a concentration of 0.003 to 0.004 mg/kg in enamel (fresh weight?).On the contrary one study from Australia reports 10 to 35 mg/kg (for dentine and enamel). More data areneeded to draw definitive conclusions.

Zinc: Zn in whole tooth appears to be in the range of 100 to 350 mg/kg. However, more results have beenreported for dentine and enamel. Based on the results from several studies from varying geographical

15

locations, the probable average concentrations appear to range anywhere from 70 to 690, and 135 to 360mg/kg, for enamel and dentine, respectively. Occasionally higher than the stated concentrations have beenreported to both the fractions. It also seems that there is a general overlap of the concentration rangesirrespective of whether fresh or dry basis has been used for expressing the results. As discussed under bone,Zn values are likely to depend on various factors such as nutrition, metabolism and environment. Good AQCprocedures have been applied by most investigators. Importantly, there is no specific analytical difficulty thatinterferes with the determination of this element in dental tissues as long as contamination from laboratoryequipment and reagents is kept under surveillance.

8. DISCUSSION

8.1 Limitations of the data compiled

With the exception of a few investigations designed with great care to blend biological and analyticalperceptions, many investigations that were reviewed during the course of this compilation suffer from a lackof interdisciplinary approach. A lack of anatomical background has frequently resulted in incompatibledescription of the samples taken for analysis. On the analytical front, to some extent the reliability of theresults have suffered due to insufficient efforts to evaluate the methods for matrix suitability. Further, thelimited availability of suitable RMs tovalidate the methods has also deteriorated the situation. Under these circumstances, it is not surprising thatthe observations resulting from several studies differ widely. Although an attempt is made in thiscompilation to identify the AQC component in a given investigation (see Tables 3 and 4), it should berecognized that these AQC observations apply mostly to the laboratory part of the work, and the fact that inmany cases the sample validity itself is questionable indicates the basic nature of the problem.

For above mentioned reasons, it is emphasized that the results compiled in this report must be used withanalytical caution and biological discretion.

8.2 Major and minor elements in bones and teeth

Bone as a matrix is rather complicated, and relating concentrations of major and minor elements to each otherhas to be done with great care. For example, when bones are properly sectioned, defatted, dried understandard working procedures and analyzed, certain postulations are valid: e.g. Ca and P are prime indicatorsof bone mineral, and N is the prime indicator of collagen and other proteins. Under well defined conditions,Ca accounts for 25 % of dry fat-free bones [1]. From an analytical point of view, assessment of Ca afterashing at moderately high temperatures is not associated with any known problems. Wet ashing is perfectlysafe for both Ca and P and many studies have reported a constant ratio for this element between differentparts of a particular bone. Na, K, and Mg can be lost during ashing at high temperatures and thus part of thevariation in the ratios is attributable to this factor. Wet ashing or cold temperature ashing is generally safefor most of the elements of this group. For S and to some extent also for K, very few studies wereencountered during this review, and even these were of doubtful quality. Therefore, for these two elements,especially for S there is very little information in this compilation. The summary information is compiled inTable 1 (Bones) and 2 (Teeth).

8.3 Trace elements in bones and teeth

Trace element studies can be classified under two groups: Pb, Sr and Zn which are extensively investigatedin bones in several countries, and others such as Al, Cd, Co, Cu, F, Fe, Mn, Rb and U. In tooth also, thetendency is similar. The summary information is compiled in Table 1 (Bones) and 2 (Teeth).

16

There are not many studies particularly looking into the distribution of trace elements within a particularhuman bone sample to localize the variations and seek a metabolic explanation, if any for such phenomenon.Braetter et al [25] have studied the distribution of Ca, F and Pb in one instance. Katie et al [31] haveexamined the temporal bone and have identified marked differences in the distribution of both structural (Ca,P and Mg) as well as the essential trace element Zn. They attribute these differences to the developmentalspecificities to be met by various regions of the bone and functional adaptation. In a Japanese studyinvestigating sex and age related variations in elemental concentrations in rib samples, a total of 20 elementswere studied [24]. Based on the analysis of rib samples from 28 male and 14 female subjects followingconclusions were drawn: Bone Fe and Pb concentrations were significantly higher, while P concentrationswere lower in males; elements Ca, P, Al, Fe, Mg, Na, Pb and Zn showed age related variations. Of these Al,Fe, Pb and Zn showed a linear relationship in accumulation with age.

In most countries Cd and Pb are considered to be priority pollutants, thus attracting more attention than restof the trace elements. As can be seen from the number of studies on Pb in bones and teeth, extreme variationsin concentrations are encountered. Obviously, living conditions greatly influence the accumulation of Pb.Age and Pb concentration in food, water and air, and the length of exposure are clearly linked to accumulationof Pb in bone and other tissues [32,33]. It is estimated that over 95 % of the Pb in the body at the age of 80will be located in the bone [34], and therefore bone (i.e. skeleton) is considered as a reliable indicator ofenvironmental exposure to Pb that can be measured in vivo by X-ray Fluorescence [35].

Grandjean and Jorgensen [18] have investigated the retention of Pb and Cd in prehistoric and modern humanteeth. In 5000 years old samples of premolars from Nubia and 500 years old samples of teeth from subjectswho had lived in Greenland, Pb concentrations were very low in comparison with modern specimens. ForCd, the results were reversed. The trend observed for Pb is explained by the excessive burdening of theenvironment with Pb, especially in the 70s and the 80s. The property of Pb to accumulate in teeth has servedas a means to monitor lead exposure of human subjects, particularly the pediatric population.

Based on Cd in cancellous bone obtained from the iliac crest, it appears that the concentration is not relatedto age [36], but specimens from male subjects showed slightly higher concentrations of Cd than those fromfemales. Interestingly, these investigators have also reported that the Cd content has a high statisticallysignificant positive correlation with Sr and Ni in the same specimens. The toxicity of Cd to bone isdocumented through the autopsy studies of itai-itai disease cases [37] revealing reduction in bone density.Similarly, subjects living in Cd polluted environment have been shown to contain elevated levels ofosteocalcin than non-exposed controls [38].

Toxicity induced by Al has become a concern. Although ingestion from food is low, prolonged exposure tofood and water can result in the accumulation of Al in bone. Consequently, excessive accumulation of Al inthe skeleton is believed to inhibit bone formation by interfering with normal bone metabolism [39]. The toxiceffect of Al on the skeleton was recognized when epidemiologic link was established between incidence ofdialysis encephalopathy and large amount of Al in the dialysate, and concomitant high incidence of fracturingosteomalacia [40]. The role of F in bone metabolism is well understood [26]. It has been extensively studiedin connection with industrial and endemic fiuorosis as well as its role as a preventive medicine for bone anddental health.

The role of Zn in bone metabolism is being increasingly appreciated. The elevated concentrations of Zn inthe urine of women with osteoporosis has been identified as a likely biomarker to screen post-menopausalwomen [41]. Saltman and Strause [34] advocate supplements of trace minerals for including Zn post-menopausal women to improve bone density. Cu is intricately linked to bone metabolism under bothdeficient and toxic conditions. Cu deficiency affects collagen metabolism while Cu toxicity is believed toinduce depletion of bone density [42]. Mn is believed to be intricately linked with bone metabolism [28], andit is suggested that supplementation of Cu, Mn and Zn may add to the beneficial effect of Ca supplementation

17

by improving the bone mineral density in post-menopausal women [34]. Not much is known about Fe inbone metabolism. Boron is gaining importance as a beneficial element for bone metabolism. It is reportedthat supplementation of basal diet low in Mg and B with 3mg/d B significantly increased plasmaconcentration of ionized Ca in women thus establishing a mode of action for B in the pathway of bonemetabolism [43].

9. CONCLUDING REMARKS

Chemical elements play a great role in the metabolism of bones and teeth. Some elements are beneficial (Fat non toxic concentrations in bones and teeth, supplementation of Cu, Mn and Zn along with Ca to delay orprevent the onset of osteoporosis) and some others (chronic exposure to Pb even at moderate concentrations,and excessive exposures to F as in fluorosis situations) are detrimental for the normal functioning of theskeleton. Knowledge on the roles played by both groups of elements can be enhanced if reliablecompositional picture is available for scrutiny.

The present survey was undertaken to assess the literature status on chemical composition of bones and teeth,and revealed that much needs to be done in order to have tangible collection of meaningful data. In thiscontext, there is a desperate need for harmonization (types of samples chosen, procedures adopted to processthe specimens, and finally the determination of analytes) to generate comparable data. To begin with, it isnecessary to develop a bioanalytical protocol that exemplifies the merits and demerits of analyzing bones andteeth.

Identification of any particular type of bone as a representative sample for the whole skeleton appears to bea far cry. Even if such a representative segment of a particular bone is identified, the logistics related tomedico-legal (autopsy) and anatomical (biopsy) parameters will prevail as decisive factors.

For the sake of gaining a comprehensive insight into the distribution of various trace elements in differenttypes of bones, it is necessary to carry out controlled investigations on different types of bones (and corticaland trabecular segments from the same sources) from the same cadaver under well defined samplingconditions.

On the analytical side, development of hard tissue RMs for whole bone, as well as for cortical, trabecular andmarrow segments separately, would be very helpful for future investigations.

18

10. REFERENCES

[I] REPORT OF THE TASK GROUP ON REFERENCE MAN, (ICRP-23), International Commissionon Radiological Protection, Pergamon Press, New York, (1975).

[2] HAMILTON, E.I., The Chemical Elements and Man. Charles C. Thomas, Spring Fields, IL, Publ.,1979.

[3] METALS IN BONE (Priest N.D. ed.) MTP Press Ltd, Boston, 1985.

[4] BIOMINERALS (Driessens F.C.M., Verbeeck, R.M.H. eds.), CRC Press, Boca Raton, FL,1991.

[5] IYENGAR, G.V., KOLLMER, W.E., BOWEN, H.J.M., Elemental Composition of Human Tissuesand Body Fluids, Verlag Chemie, Weinheim, New York, (1978).

[6] IYENGAR, G.V., Elemental Analysis of Biological Systems, Vol. I, CRC Press, Boca Raton, Fl,(1989).

[7] JOHNSON, L.C., Morphographic analysis in pathology. In, Bone Biodynamics, Frost, H.M., (ed),Little Brown, Boston, 1964, Chapter 29, pp. 543-654.

[8] PARFITT, A.M., The physiologic and clinical significance of bone histomorphometric data. In, Bonehistomorphometry: Techniques and Interpretation, ed. By R.R. Recker, Boca Raton, Fl, (1983), pp.143-223.

[9] ARNOLD, J.S., BARTLEY, M.H., TONT, S.A., JENKINS, D.P., Skeletal changes in aging anddisease. Clin. Orthop. Relat. Res., 49(1966) 17-38.

[10] BOHR, H., SCHAADT, O., Bone mineral content of the femoral neck and shaft: Relation Betweencortical and trabecular bone. Calcified Tissue Int. 37 (1985)340-344.

[II] ROBINSON, R.A., Chemical analysis and electron microscopy of bone. In, Bone as a Tissue, Rodhal,IT, , Nicholson, E.M. (Eds), McGraw Hill, New York, (19600), pp.

[12] GONG, J.K., ARNOLD, J.S., COHN, S.H. Composition of trabecular and cortical bone. Anat. Res.,149(1964)325-331.

[13] BLANTON, P.L., BIGGS, N.L. Density of fresh and embalmed human compact and cancellous bone.Am. J. Phys. Anthrop., 29(1968) 39-44.

[14] GAWLIK, D., BEHNE, D., BRAETTER, P., GATSCHKE, W., GESSNER, H.5 KRAFT, D., Thesuitability of the Iliac crest biopsy in the element analysis of bone and marrow. J. Clin. Chem. Clin.Biochem. 20(1982) 499-507.

[15] INSKIP, M.J., FRANKLIN, C.A., SUBRAMANIAN, K.S., BLENKINSOP, J. WANDELMAIER,F., Sampling of cortical and trabecular bone for lead analysis: Method development in a study of leadmobilization during pregnancy. Neuro Toxicology 13(1992)825-834.

[16] EASTOE, J.E., The chemicalcomposition of teeth. In, Biochemist's Handbook, Long, C , (ed) D. VanNostrand Co, New York, (1961), pp. 720-724.

19

[17] FERGUSSON, J.E., PURCHASE, N.G., The analysis and levels of lead in human teeth. Environ.Pollution 46(1987)11-44.

[18] GRANDJEAN, P., JORGENSEN P,I, Retention of lead and cadmium in prehistoric and modernhuman teeth. Environ. Res. 53 (1990) 6-15.

[19] CUA, F.T., HALL, G.S. Trace element analysis of human teeth and bone by proton Induced X-rayemission. Biol. Trace Ele. Res. 12(1987) 133-142.

[20] ZWANZIGER, H., The multi elemental analysis of bone: A review Biol. Trace Ele. Res. 19 (989) 195-232.

[21] SUBRAMANIAN, K. S., CONNOR J.W., MERANGER, J.C., Bone lead analysis: Development ofanalytical methodology for milligram samples. Arch. Environ. Contain, and Toxicol. 24(1993)494-497.

[22] IYENGAR, G.V., KASPAREK, K., Application of brittle fracture technique (BFT) to homogenizebiological samples and some observations regarding the distribution behavior of trace elements atvarious concentration levels in a biological matrix. J. Rational. Chem. 39(1977)301-316.

[23] EDWARD, J.G, BENFER, RA., MORRIS, J.S. The effects of dry ashing on the Composition ofhuman and animal bone. Biol. Trace Ele. Res. 25(1990) 219-231.

[24] YOSHINAGA, J., SUZUKI, T., MORITA, M. Sex and age related variation in elementalconcentrations of contemporary Japanese ribs. Sci. Total Environ. 79(1989)209-221.

[25] BRAETTER, P., GAWLEK, D., ROESICK, U., A view into the past: Trace element analysis of humanbone from former times. HOMO, Vol. 39 (1987), Book 2, pp 99-106.

[26] KRISHNAMACHARI, K.V.R.V., Fluoride. In, Trace Elements in Human and Animal Nutrition,(Mertz, W. Ed.) Academic Press, New York, Volume 1, 1986, pp. 365-407.

[27] SUBRAMANIAN, K. S. Lead. In, Quantitative Trace Analysis of Biological Materials, McKenzie,H.A., Smythe, L.E. eds.), Elsevier Publ, Amsterdam, 1988, pp. 589-603.

[28] STRAUSE, L. , SALTMAN, P., Role of Manganese in bone metabolism. Chapter 5, In NutritionalBioavailability of Manganese, (Kies, C, ed.), ACS Symp. Series 354, Washington D.C., 1987, pp.46-55.

[29] HURLEY, L.L. Manganese, In, Trace Elements in Human and Animal Nutrition, (Mertz, W. Ed.)Academic Press, New York, Volume 1,1986, pp. 185-215.

[3 0] CUTRESS, T. W., A preliminary study of the micro element composition of the outer layer of dentalenamel. Caries Res. 13(1979)73-79.

[31] KATIC, V., VUJICIC, G., IVANKOVIC, D., STAVLJENIC, A., VUKICEVIC, S., Distribution ofstructural and trace elements in human temporal bone. Biol. Trace Ele. Res. 29(1991)35-43.

[32] SAMUELS, E.R., MERANGER, J.C., TRACY, B.L., SUBRAMANIAN, K.S. Lead concentrationsin human bones from the Canadian population. Sci. Total Environ. 89(1989)261-269.

20

[33] BEATTIE, J.H., AVENELL, A., Trace element nutrition and bone metabolism. Nutr. Res. Reviews5(1992)167-188.

[34] SALTMAN, P., STRAUSE, L. The role of trace minerals in Osteoporosis. J. Am. College ofNutrition 4(1993)384-389.

[35] NORDBERG, G.F., MAHAFFEY, K.R., FOWLER, B.A., Lead in bone: Implications for dosimetryand toxicology. Environ. Health Persp. 91(1991)3-7.

[36] KNUUTTILA M., LAPPALAINEN, R., OLKKONEN H., LAMML S., ALHAVA, KM. Cadmiumcontent of human cancellous bone. Arch. Environ. Health 37(1982)290-294.

[37] NODA, M., KITAGAWA, M., A quantitative study of iliac bone histopathology on 62 cases with itai-itai disease. Calcified Tissue International 47(1990)66-74.

[38] KIDO, T., HONDA, R., TSURITANI, I., ISHIZAKI, M., YAMADA, Y., NAKAGAWA, H.,NOGAWA, K., DOHI, Y. Serum levels of bone Gla-protein In inhabitants exposed environmental Cd..Arch. Environ. Health 46(1991)43-49.

[39] RODRIGUEZ, M., FELSENFELF, A. J., LLACH, F., Aluminum administration in the rat separatelyaffects the osteoblast and bone mineralization. J. Bone and Mineral Res. 5(1990)59-67.

[40] ALFREY, A.C., Aluminum. In, Trace Elements in Human and Animal Nutrition, (Mertz, W. Ed.)Academic Press, New York, Volume 2,1986, pp. 399-409.

[41] HERZBERG, M., FOLDES, J., STEINBERG, R., MENCZEL, J. Zinc excretion in osteoporoticwomen. J. Bone and Mineral Res. 5(1990)251-257.

[42] SAYMOUR, C.A., Copper toxicity in man. In Copper in Animals and Man. (MaC Howell, J.,Gawthrone, J.M. Eds.)CRC Press, Boca Raton, FL, 198, pp. 79-106.

[43] NIELSEN, F.H., SHULER, T.R., ZIMMERMAN, T.J., UTHUS, E.O. Effect of boron depletion andrepletion on blood indicators of Ca status in humans fed a magnesium low diet. J. Trace Ele. In Exp.Med., 3(1990)45-54.

21

ANNEXES (Data compilation)

22

Table 1:Range of Mean Values

ElementAg (mg/kg)

Al (mg/kg)

As (mg/kg)

Au (mg/kg)

B (mg/kg)

Ba (mg/kg)

Be (mg/kg)

Bi (mg/kg)

Br (mg/kg)

Ca(%)

Cd (mg/kg)

Cl (mg/kg)

Co (mg/kg)

Cr (mg/kg)

Cs (mg/kg)

Cu (mg/kg)

Eu (mg/kg)

F (mg/kg)

Fe (mg/kg)

Hg (mg/kg)

I (mg/kg)

K (mg/kg)

La (mg/kg)

Li (mg/kg)

Mg (%)

Mn (mg/kg)

Mo (mg/kg)

N (%)

Na (%)

Nb (mg/kg)

Ni (mg/kg)

O(%)

P(%)

Pb (mg/kg)

for Major, Minor and Trace Elements i[yengar et

Sample

Prep

a

a

a

a

f

a*

a

f*

a

f*

*

f*

*

*

af

f

a

*

*

a

*

*

a

*

f

al.,1978 (Pre-1978)

Range

1.1

30 - 66.74.1

<0.030.74 - 0.97.4 - 29

< 0.0002 - < 0.001<0.2

38

17-27.44.2

632

0.01 - 0.0290.1-33

0.009 - 0.0361.0-25.7

654-61803-40<0.7

15

1470<0.2

0.070 - 0.0980.19-3

103

0.560-1.41

<0.07110

10.3 - 17.410-42.5

n Human BonesPresent Literature Values

Sample

Prep

a

d

a

f

f

d

f

d

d

d

d

d

a

d

a

d

d

d

d

d

d

d

a

d

d

f

f

d

d

Range

0.041 - 0.061

1.81-45.60.0011<0.5

8

2.7 -5.93

1.4 - 12.48.62 - 28.9

0.0247 - 2.2228 - 2700

0.0153-0.132.75 - 10.8

0.046 - 0.0760.19-22.6

0.024 - 0.029639-210831.2-532.50.018 - 0.62

47.9 - 6220

0.230.01 -0.390.14-7.6

0.065 - 0.0664.49 - 5.05

0.316-0.805

0.42-9.1230 -45.67.1 -12.5

0.57 - 70.66

23

Element

Po (mg/kg)

Ra(mg/kg)

Rb (mg/kg)

S (mg/kg)

Sb (mg/kg)

Sc (mg/kg)

Se (mg/kg)

Si (mg/kg)

Sn (mg/kg)

Sr (mg/kg)

Ta (mg/kg)

Tb (mg/kg)

Th (mg/kg)

Ti (mg/kg)

Tl (mg/kg)

U (mg/kg)

V (mg/kg)

W (mg/kg)

Y (mg/kg)

Zn (mg/kg)

Zr (mg/kg)

Iyengar et alSample

Prep

a***

f*

*

aa

a

f

a

a*

*

*

a

.,1978 (Pre-1978)

Range

(5.9-260)xl0"12

(10-12.5)xl0"9

0.1-5.11500

0.01-0.34.6

1 - 8.9517

3.9

90.2 - 172

0.005 - < 0.04

0.0020.0004 - 0.02

1.20.00025

0.0750 - 170

<0.1

Present Literature ValuesSample

Prep

W

W

d

d

d

d

d

d

d

a

aad

w

d

d

a

Range

(7.7 - 8.78) x lO'12

1.09 xlO"9

< 0.04 - 37.6800

0.01510.0014 - 0.092

0.13-0.56

2.3

48.1-4180.04 - 0.047

0.013 - 0.03440.24 - 0.381.95-< 5.0

0.00055 - < 0.5<2.0-<6.0

91 -265.842.69 - 44.30

a = ashed

d = dry weight

f = freeze dried

n = no sample preparation

w = wet weight

* not clear or not addressed

24

Table 2:Range of Mean Values for Major, Minor and Trace Elements in Human Teeth

Dentine Enamel Whole Tooth1

Reference

Sample

Prep Range

Sample

Prep Range

Sample

Prep Range

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Att&Bg&g)

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

lyengar et al.,1978 (Pre -1978)

0.004 -2.2

0.08

62 -136

0.022 - 0.1

0.03 - 0.07

• 0.005 - 0.56

* 0.06-32

12.5 - 86

2.1-343

• < 0.02-0.07

* <14

<0.0001-0.11

* 129

* 25

* 4.2-114

* 25.0-28.2

* 31.5

* 0.099-0.12

* 0.086 0.097

**

*

*

*

*

*

*

•

*

*

*

*

*

5

0.87 - 8.40

4.2 -125

2.02 - 22

<0.01

1.3-1.36

0.006

0.001

1.12-34

3.1

36.0-37.4

31.5-37.34

< 0.0001-0.51

0.03-9.1

0.07

4.12

9.97-11.7

1.7-4.2

25

Dentine Enamel Whole Tooth1

Reference

Sample

Prep Range

Sample

Prep Range

Sample

Prep Range

Present Literature Values

yengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

yengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

lyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

350-3900

0.6

• 3200 - 6500

* 7900 - 8900

* 0.006-1.11

* 0.1

• 0.005-2

* 0.21-28

• 3

**

•

*

*

*

*

d

0.004-0.13

0.2 - < 16

0.005 - 3.2

0.45 - < 34

0.04

0.1

0.26-33

0.21-282

<0.09

<0.04

140-

31.7-

157

110

**

*

*

293-2640

54.3-752

4.4 - 338

27.95 -138

<0.02

6

< 0.08

* <0.02

* 7.6

4.8-24.8

42.6-47.2

6.8 - 9.76

32.03-65

26

Dentine Enamel Whole Tooth1

Reference

Sample

Prep Range

Sample

Prep Range

Sample

Prep Range

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

670

<0.08

<0.11-3.15

22

<0.02

0.036

0.05-2.04

<0.04

••

*

*

*

*

401

191.04-1200

<0.02

1.4

1.13

0.53 -14

<0.02

* 6180-8700

* 7926

* 0.19 -10.5

* 3.9

* 2.3

**

*

*

*

*

1670-2800

745-4100

0.28 - 30

0.60 - 59

0.054 -7.2

0.1-2.37

0.2

53.3 - 53.47

9.06-47.65

27

Dentine Enamel Whole Tooth1

Reference

Sample

Prep Range

Sample

Prep Range

Sample

Prep Range

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

28

5300-7500

1.35

0.9

<0.09

12.1-13.5

14

7.3 - 52

1.55-149.3

5.7

0.008

9 - 86.5

* 3900-11600

* 13600

0.28

0.17

0.045

0.29-23

10.0-18.3

16.1-21

3.6 - 36

1.7-1236

<0.05

0.027

0.2

<90

0.39-73

1126-1193

4.6-31.3

1.65-53.5

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre- 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

500 - 670

0.69 - 0.7

12.8

78-138

93

70 -100

75 -136.7

0.15-4.61

<0.04

<0.01

<0.04

48-281

24.19-18780

0.078 - 0.96

0.02- 8

<0.1

0.27-0.872

1.47-18

60

70

<0.08

0.21 -120

1.60-< 325

81-111

81.51-206.4 23

<0.02

29

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre - 1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

Iyengar et al.,1978 (Pre -1978)

Present Literature Values

11-23

0.0047

0.007 - 0.034

2.6

0.19

1.6-1.93

<0.04

<0.02

< 0.01-0.017

0.0031 -1.4

0.24

<325

< 0.007

1.8

* 173

* 135.1

-250

-359.3

**

*

*

199-366

69.7 - 893

0.1

0.08

103-357

1 = Whole tooth or regions not separated orspecified

d = dry weight basis

n = no sample preparation

* not clear or not addressed at present

30

Table 3:Notations used in BoneCompilation

a = ashed

d = dry weight

f= freeze dried

m = macerated

w = wet weight

c = cortical

cm — concha media

ci = concha inferior

cl = cancellous

e = ethmoid

m = metatarsal

ma = maxilla

of= osfrontale

os = os parietale

pm = processus mastoides

r/u = radius/ulna

s = septum

t = trabecular

tb = tibia

tbf= tibia fragment

tbs = tibia section

te = temporal

AAS = atomic absorption spectrometry

C = colorimetiy

CPAA = charged particle activation analysis

EDX = energy-dipersive x-ray microanalysis

FT = fission track method

IGAA = instrumental gamma-activation analysis

ICPAES = inductively-coupled plasma atomic emission spectrometry

ICAP = inductively-coupled argon plasma

ICPMS = inductively-coupled plasma mass spectrometry

ISE = ion-selective electrode

LF = laser fluorimetry

MS = mass spectrometry

N = nitrogen analyzer

NAA = neutron activation analysis

PKE = proton induced x-ray emission

PIGE = proton induced gamma-ray emission

PGAA = prompt-gamma activation analysis

RAD = radiochemical methods

31

RBS = Rutherford backscattering spectrometry

XRF = x-ray fluorescence

V = voltametry

ICS = in-house calibration standard

L = no QA/QC mentioned but agreement with the literature values

L*= Lianqing and Guiyun, 1990

Z* = Zwanziger, 1989

32

Maior. Minor, and Trace Element in Human Bones (IAEA Compilation Post 19781

Reference

Bush etal., 1995

Yoshinagaetal., 1989

Kosugi et al., 1988

Mahanti and Barnes, 1983

Gawlik etal., 1982

Hyvonen-Dabek, 1981

Yoshingaetal., 1995

Zaichick, 1994

Pietra et al., 1993

Lin and Wen, 1988

Location

Japan

Japan

Japan

Italy

China

Age

yrs.

18-85

0.17-82

24-70

>10

Sample

Preparation

d

d

d

a

d

f

d

d

w

a

Range

0.242 -14.21 (c)

<22-54

0.0023-0.012

Mean

1.81 ± 2.58 (c)

41.0 ±20.6

45.6 x/, 1.3

42.9 ±0.8

19.5 ±6.1

<22

0.47 ±0.20

0.061 ± 0.063 (M)

0.041 ± 0.029 (F)

Median

<0.4

Number of

Samples

30

(18M.12F)

42

(28M.14F)

18

11M.7F

3

15

35

18, M

17 F

Analytical

Technique

ICPMS

ICPAES

ICPAES

ICPAES

NAA

PIGE

ICPMS

NAA

NAA

NAA

33

Reference

Yoshinga et al., 1995

Pietraetal., 1993

Mahanti and Bames, 1983

Yoshinga etal., 1995

Pietra et al., 1993

Huntinetal., 1982

Kosugi et al., 1988

Ward, 1987

HyvSnen-Dabek, 1981

Yoshinga et al., 1995

Location

Japan

Italy

Japan

Italy

Japan

New Zealand

Japan

Age

JTS.

69-84

24-70

Sample

Preparation

d

w

a

d

w

f

d

d

f

d

Range

<0.1-0.S

< 0.002-0.010

0.00003-0.00039

<2-14

0.41-3.20

Mean

0.011 ±0.0005

<0.5

<0.5

23.4 x/, 3.3

19.79 ±4.18

8.0 ±3.3

Median

<0.1

<0.1

1.3

Number of

Samples

35

3

35

10

18

11M.7F

14

15

35

Analytical

Technique

ICPMS

NAA

ICPAES

ICPMS

NAA

V

ICPAES

PGAA

PIGE

ICPMS

34

Reference

Kniewald et al., 1994

Pietraetal., 1993

Samudralawar and Robertson, 1993

Manea-Krichtenetal., 1991

Zwanziger et al., 1987 & 1985

Jaworowski et al., 1985

Mahanti and Bames, 1983

Yoshinga et al., 1995

Robertson et al., 1992

Samudralawar and Robertson, 1993

Grynpas et al., 1987

Smytheetal.,1982

Hyvanen-Dabek et al., 1981

LocationCroatia

Italy

USA

USA

France

Japan

USA

USA

Australia

Age

yrs.

60-82

67-96

34-89

60-82

60-82

3 - 80 (80%)

Sample

Preparationfw

f

d

d?

d

a

d

f

f

d

d

f

Range148.6-190.1

1.7-3.4

3.53 -14.6

2.82 -14.6

17-314

< 0.5 -15

1.1-12.8 (c)0.5-2.7(0

5.46 - 20.3 (n = 7)

Mean

36 ± 13 (c)

19±7(c/)

5.93 ± 4.37

5.76 ±4.50

2.7 ±3.9

21.0 ±0.4

4.1 ± 4.0 (c)1.4 ±0.6(0

1.4±0.6(cQ

110±55(c)

290 ±60 (del)

180±60(cQ

10.3 ±4.5

12.4 ±5.5

Median

35.0

18

<0.2

3.0

1.2

1.2

Number of

Samples5

5

4

6 (2M.4F)

22?

3

35

12

8M.4F

12

8M.4F7

8

8

7

15

9M.6F

Analytical

Technique

ICPAES

NAA

PKE

MS

NAA

ICPES

ICPAES

ICPMS

PKE

PKE

NAA

XRF

PKE

35

Reference

Bush etal., 1995

Yoshingaetal., 1995

Akesson etal., 1994

Kniewald etal., 1994

Zaichick, 1994

Samudralawar and Robertson, 1993

Robertson et al., 1992

Katie etal., 1991

Manea-Krichten et al., 1991

Edward, 1990

Hisanaga et al., 1989

Yoshinagaetal., 1989

Hisanaga et al., 1988

Kosugietal., 1988

Grynpas et al., 1987

Location

Japan

Croatia

USA

USA

USA

Japan

Japan

Japan

Japan

Age

yrs.

18-85

61-96

40-76

60-82

60-82

36-77

67-96

65

40-60

0.17-82

40-60

Sample

Preparation

d

d

d?

fd

f

f

d

d

w

d

r~~ d

d

d

d

Range

12.2-35.8 (c)

57.5-61.0

12.6 - 27.5 (c)

14.8-22.2(023.2-30.1 (fe)

23.4-25.9

22.3-25.4

15.3 -18.8

Mean

22.2 ± 4.4 (c)

24.6 ±0.6

25.8 ±0.7(0

22.2 ± 0.5 (0

23.0 ±1.0(0

22.6 ±2.1

19±2.2(cQ

20 ±4.1 (c)

19 ±2.4 (t)

26.7 ±2.3 (te)

24.6 ±1.1

24±1

23.5 ±0.2

16.8 ±1.3

23.9 ±0.9

16.8 ±1.3

16.7 x/, 0.012

22.5 ± 1.4 (c)

Median

24.7

19.0

21

19

24

Number of

Samples

30

30 (18 M, 12 F)

45

17M.28F

5

3M.2F

5

12

8M.4F

12

8M,4F

174

6 (2M, 4F)

1,M

11

42

(28M.14F)

11

18

11M.7F

7

Analytical

Technique

ICPAES

AAS

& ICPAES

EDX

NAA

ICPES

ICPAES

NAA.XRF

IGAA

PIXE

PKE

ICPAES

MS

NAA

AAS

AAS

AAS

ICPAES

NAA

36

Reference

Igarashietal., 1987

Zwanziger et al., 1987 & 1985

Jaworowski et al., 1985

Mahanti and Barnes, 1983

Niebergalletal., 1983

Gawliketal., 1982

Niese et al, 1982

Smythe et al., 1982

Hyvönen-Dabek, 1981

Lindh, 1981

Eichhorn et al., 1980

Giarratano et al, 1979

Hyvönen-Dabek, 1979

Location

Japan

France

Australia

Age

JTS,

37-94

34-89

3 - 80 (80%)

24-70

65

Sample

Preparation

w

d ?

d

a

d ?

d

d ?

d

f

d

d ?

worf?f

Range

14-19

4.1 -12

5.0 -13.0

6.4-28.7

7.3-22.6

18.4-23.1

Mean

18.6 ± 2.8 (del)

15.5 ± 3.0 (et)

17±2

7.9 ±2.5

8.7 ±2.7

18.5 ±3.4

27.1 ±0.3

29.4

21.3 ±0.1

24.51 (op)

25.53 (pm)

25.95 (ofi

8.62 ±2.52

20.4 ±1.3

25.58

28.9 ±11.5

7.25 ± 1.06

38.6 ± 0.7 (M)

37.5 ± 0.8 (F)

37.1 ± 0.9 (M)

37.8 ± 0.3 (F)

Median

Number of

Samples

8

8

6

3M.3F

7

4M.3F

7

4M.3F

22?

3

3

7

15

IM

1

8M

3 F

8M

3 F

Analytical

Technique

ICPAES

ICPAES

ICPAES

NAA

ICPES

ICPAES

ICAP

NAA

NAA

XRF

PIGE

PEXE

NAA

NAA

RBS

37

Reference

Bush etal., 1995

Baranowska et al , 1995

Yoshinga et al , 1995

Kniewald etal , 1994

Pietra etal , 1993

Samudraiawar and Robertson, 1993

Saltzman et al , 1990

Hisanaga et al , 1989

Yoshinagaetal, 1989

Kosugi et al , 1988

Jaworowski et al , 1985

Knuuttilaetal, 1982

Liese, 1982

Location

Poland

Japan

Croatia

Italy

USA

USA

Japan

Japan

Japan

France

Age

yrs.

18-85

26-55

61-96

60-82

20-74

40-60

0.17-82

34-89

Sample

Preparation

d

f

d

fw

f

w

d

d

d

d

m

d

d?

Range

0-0.12(e)

0.05 -1.5

0.05 - 0.38

> 0.001-0.053

0.110-0.640

0.07 - 8.0

Mean

0.029 ± 0.03 (c)

0.69 ±0.38

0.14 ±0.10

0.28 ± 0.62

2.7 ± 1.0 (c)

2.4 ± 1.2 (ct)

0.07 ± 0.07 (M)

0.11 ±0.13 (F)

0.06 ± 0.06 (M)

0.08 ± 0.06 (F)

0.05 ± 0.05 (M)

0.06 ± 0.03 (F)

0.03 ± 0.04 (M)

0.03 ± 0.02 (F)

0.57 ±0.26

0.09 ±0.10

0.06 x/, 5.9

2.2 ±2.2

0.24 ±0.17 (M)

0.21 ± 0.16 (F)

0.0247

Median

<0.1

2.5

2.6

<0.1

Number of

Samples

30

30 (18 M, 12 F)

25 (15 M, 10 F)

10 (7M, 3 F)

45

17M.28F

5

5

4

21 M

5F

21 M

5F

21 M

5F

21 M

5F

11

18

18

11M,7F

22?

88

61M.21F

30

Analytical

Technique

AAS

AAS

AAS

&ICPAES

V

NAA

PKE

AAS

AAS

ICPAES

ICPAES

AAS

AAS

V

38

Reference

Zaichick, 1994

Edward, 1990

Grynpas et al., 1987

Zwanziger et al., 1987 & 1985

Nieseetal., 1982

Lindh, 1981

Giarratano et al., 1979

Yoshingaetal., 1995

Zaichick, 1994

Pietra et al., 1993

Yoshinaga et al, 1989

Kosugi et al, 1988

Location

Japan

Italy

Japan

Japan

Age

yrs.

65

65

61-96

0.17-82

Sample

Preparation

d

w

d

d?

d ?

d

worf?

d

d

w

d

d

Range

458-1197

0.044-0.073

Mean

1210 ±320

934.0 ±17.0

1300 ± 300 (c)

2700 ± 800 (del)

1600 ± 600 (cl)

262 (op)

356 iptri)

228 (of)

800

2070 ± 665

0.08 ±0.05

0.0153 ±0.0029

0.12 ±0.12

0.06 x/, 1.4

0.13 x/, 2.0

Median

<0.1

<0.1

Number of

Samples

1,M

7

8

8

1M

1

45

17M.28F

-

8

11(7M,4F)

7(4M,3F)

Analytical

Technique

NAA

NAA

NAA

NAA

NAA

PKE

NAA

AAS

&ICPAES

NAA

NAA

ICPAES

ICPAES

39

ReferenceLin and Wen, 1988

Zwanziger et al, 1987 & 1985

Gawliketal., 1982

Mahanti and Barnes, 1983

Yoshinga et al, 1995

Zaichick, 1994

Pietra et al, 1993

Samudralawar and Robertson, 1993

Yoshinagaetal, 1989

Kosugietal, 1988

Lin and Wen, 1988

Hyv6nen-Dabek et al, 1981

Yoshinsaetal., 1995

LocationChina

Japan

Italy

USA

Japan

Japan

China

Japan

Age

yrs.>10

61-96

60-82

0.17-82

>10

24-70

Sample

Preparationa

d ?

d

a

d

d

w

f

d

d

a

f

d

Range

0.48-3.84

0.710-2.450

1.5-2.3(n = 3)

Mean0.62 ± 0.52 (M)

0.48 ± 0.46 (F)

0.046 ±0.037

0.4 ±0.01

<6.0

2.75 ±0.75

1.8 ± 0.7 {c)

1.9±0.8(cQ

4.87 ±1.14

10.8 x/, 1.1

11.58 ±11.19 (M)

5.72 ± 3.45 (F)

<2.0

Median

<6.0

3.0

3

4.88

< 0.004

Number of

Samples23, M

24, F

3

45

17M.28F

5

4

38

18

11M,7F

21, M

22, F

15

9M.6F

35

Analytical

TechniqueNAA

NAA

NAA

ICPAES

AAS

& ICPAES

NAA

NAA

PKE

ICPAES

ICPAES

NAA

PDCE

ICPMS

40

Reference

Pietra et al., 1993

Lin and Wen, 1988

Baranowskaetal., 1995

Bushetal., 1995

Yoshinga et al., 1995

Pietra etal., 1993

Samudralawar and Robertson, 1993

Robertson et al, 1992

Katie etal., 1991

Saltzman et al., 1990

Hisanaga et al, 1989

Location

M y

China

Poland

Japan

Italy

USA

USA

USA

Japan

Age

yrs.

>10

26-55

18-85

61-96

60-82

60-82

36-77

20-74

40-60

Sample

Preparation

w

a

f

d

d

w

f

f

d

w

d

Range

0.0295-0.056

0.18-5.17

0.19-0.50

0.5.0 (c)

0.790-2.148

<0.7-32.3 (c)

< 0.7 - 47 (t)

14-30(fe)

Mean

0.076 ± 0.048 (M)

0.046 ± 0.013 (F)

0.70 ±1.10

0.31 ±0.10

1.0 ± 1.3 (c)

0.19 ±0.20

6.3 ± 9.2 (c)

1.4±4.1(cQ

5.1 ± 9.2 (c)

4.8 ±13(f)

20.5 ± 9.2 (fe)

0.41 ± 0.15 (M)

0.44 ± 0.15 (F)

0.34 ± 0.18 (M)

0.29 ± 0.18 (F)

0.39 ± 0.22 (M)

0.52 ± 0.39 (F)

0.38 ± 0.15 (M)

0.35 ± 0.07 (F)

3.41 ±0.71

Median

<0.3

1.2

0.7

1.2

0.7

Number of

Samples

17, M

13, F

25 (15 M, 10 F)

10 (7M, 3 F)

30

30 (18 M, 12 F)

45

17M,28F

13

13

11

6

77

21 M

5F

21 M

5F

21 M

5F

21 M

5F

11

Analytical

Technique

NAA

NAA

AAS

ICPAES

AAS

& ICPAES

NAA

PIXE

PDCE

ICPAES

AAS

AAS

41

Reference

Yoshinaga et al., 1989

Kosugi et al , 1988

Jaksic et al , 1987

Mahanti and Barnes, 1983

Lappalainen et al, 1982

Smytheetal, 1982

HyvSnen-Dabeketal, 1981

»?£«)#&$ -

Yoshinga et al, 1995

Yoshinga et al , 1995

Location

Japan

Japan

Australia

Japan

Japan

Age

yrs.

0.17-82

66

3 - 80 (80%)

24-70

Sample

Preparation

d

d

m

a

d?

d

f

d

d

Range

1.78-8.00 (n =14)

< 0.01-0.06

< 0.01-0.04

Mean

0.23 ±0.22

22.6 x/, 1.1

8.64 x/. 2.0

6 (ma)

Hs)

5 (cm)

7 (ma)

12 (e)

19 (ci)

16 (cm)

1.0 ±0.03

1.3 ±0.5

1.5 ±0.8

3.58 ±2.16

Median

<0.3

<0.01

<0.01

Number of

Samples

38

11(7 M.4F)

7(4M,3F)

3

304

4

33

4

4

3

13887M.51F

3

15

9M.6F

35

35

Analytical

Technique

ICPAES

ICPAES

XRF

PEXE

ICPAES

AAS

XRF

PKE

ICPMS

ICPMS

42

Reference

Yoshinga et a!., 1995

Lin and Wen, 1988

Zaichick, 1994

Samudralawar and Robertson, 1993

Robertson et al., 1992

Gawlik et al., 1982

Hyvdnen-Dabek, 1981

Suzuki et al., 1979

Yoshinga etal., 1995

Location

Japan

China

USA

USA

Japan

Age

yrs.

>10

60-82

60-82

24-70

61-96

Sample

Preparation

d

a

d

f

f

d

f

d

a

d

a

d

Range

1030-4360 (c)

731-3419(0

178-1630

Mean

0.029 ± 0.022 (M)

0.024 ± 0.012 (F)

510±10

1710 ± 632 (cl)

2108 ± 940 (c)

1947 ±741(0

626 ±573

639 ±417

610

1100

530

960

71.0 ±64.2

Median

< 0.008

1624

1769

1864

50

Number of

Samples

35

23, M

22, F

12

8M.4F

12

8\^4F

15

45

17M.28F

Analytical

Technique

ICPMS

NAA

IGAA

PKE

PIGE

NAA

PIGE

AAS

&ICPAES

43

Reference

Bush etal., 1995

Zaichick, 1994

Pietra etal., 1993

Samudralawar and Robertson, 1993

Robertson et al., 1992

Katie etal., 1991

Hisanaga et al., 1989

Yoshinaga et al., 1989

Kosugi et al., 1988

Lin and Wen, 1988

Igarashi et al., 1987

Jaksic etal., 1987

Location

Italy

USA

USA

Japan

Japan

Japan

China

Japan

Age

yrs.

18-85

60-82

60-82

36-77

40-60

0.17-82

>10

37-94

66

Sample

Preparation

d

d

w

f

f

d

d

d

d

a

w

m

Range

9.0 -126 (c)

180-778

5.1- 39 (c)

15-144(f)

92 -124 (te)

8.6-35

94-410

1.9-26.0

Mean

54±31.8(c)

59 ±17

77±46(cQ

23±ll(c)71 ±45(0

105.6 ± 16.3 (te)

532.5 ±213.0

31.2 ±41.3

104 W1, 1.8

1000 ± 1300 (M)

630 ± 350 (F)

23±9

240 ±140

13±9

361 (ma)

360 (e)

374 (s)

624 (a)

642 (cm)

Median

73

21

73

16.3

Number of

Samples

30

30 (18 M, 12 F)

12

8M,4F

12

8M.4F

77

11

34

18

11M.7F

23, M

24, F

6

3M,3F

7

4M.3F

7

4M,3F

33

304

4

Analytical

Technique

ICPAES

NAA

&XRF

NAA

PKE

PKE

ICPAES

AAS

ICPAES

ICPAES

NAA

ICPAES

ICPAES

ICPAES

XRF

44

Reference

Zwanziger et al., 1987 & 1985

Mahanti and Barnes, 1983

Gawliketal., 1982

Hyv6nen-Dabek et al., 1981

O'Connor et al., 1980

Yoshinga et al., 1995

Yoshinga et al., 1995

Location

Australia

Japan

Japan

Age

yrs.

24-70

20-77

Sample

Preparation

d ?

a

d

f

a

d

d

Range

50-345

4.97-10.4

522 - 2164

< 0.008-0.2

Mean

690 (ma)

740 (e)

878 (ci)

934 (cm)

29.4 ±0.6

183 ±78

7.58 ±1.55

1098 ±411

Median

<0.03

< 0.008

Number of

Samples

33

4

4

3

15

9M,6F

33

21M.12F

35

35

Analytical

Technique

PKE

NAA

ICPAES

NAA

PKE

XRF

ICPMS

ICPMS

45

Reference

Yoshinga et al., 1995

Yoshinga et al., 1995

Bush etal., 1995

Zaichick, 1994

Mahanti and Bames, 1983

Yoshinga etal., 1995

Yoshinga et al., 1995

Yoshinga etal., 1995

Location

Japan

Japan

Japan

Japan

Japan

Age

vrs.

18-85

61-96

Sample

Preparation

d

d

d

d

a

d

d

d

Range

< 0.2-0.6

0-0.110(c)

< 0.01-0.01

Mean

0.018 ± 0.02 (c)

0.62 ± 0.29

0.012 ±0.0003

47.9 ± 15.2

Median

<0.07

<0.2

< 0.004

<0.01

43.5

Number of

Samples

35

35

30

30 (18 M, 12 F)

3

35

35

45

Analytical

Technique

ICPMS

ICPMS

AAS

NAA

ICPAES

ICPMS

ICPMS

AAS

46

Reference

Yoshinaga et al., 1989

Kosugi et al., 1988

Smytheetal., 1982

Panday et a l , 1980

Yoshinga et al., 1995

Yoshinga et al., 1995

Knuuttilaetal., 1982

t*J$ngftg>

Yoshinga et al., 1995

Pietraetal, 1993

Location

Japan

Japan

Australia

Japan

Japan

Japan

Italy

Age

yrs.

0.17-82

3 - 80 (80%)

Sample

Preparation

d

d

d

d

w

d

d

d ?

d

w

Range

< 0.3 -1.0

0.0049-0.014

Mean

80.7 ±58.2

429 x/, 1.9

87.2 x/, 1.6

6220 ± 569

4190

1300

0.23

Median

62.8

<0.3

<0.05

< 0.004

Number of

Samples

17M.28F

42

28M.14F

11(7M,4F)

7(4M,3F)

7

35

35

35

Analytical

Technique

&ICPAES

AAS

AAS

XRF

NAA

ICPMS

ICPMS

AAS

ICPMS

NAA

47

Reference

Bush etal., 1995

Yoshinga et al., 1995

Akessonetal, 1994

Zaichick, 1994

Samudralawar and Robertson, 1993

Robertson et al., 1992

Katie etal., 1991

Edward, 1990

Yoshinaga et al., 1989

Kosugi etal., 1988

Grynpas et al., 1987

Zwanziger et al., 1987 & 1985

Jaworowski et al., 1985

Mahanti and Barnes, 1983

Niebergall et al., 1983

Niese et al., 1982

Location

Japan

USA

USA

Japan

Japan

France

Age

yrs.

18-85

61-96

40-76

60-82

60-82

36-77

65

0.17-82

34-89

Sample

Preparation

d

d

d ?

d

f

f

d

w

d

d

d

d?

d

a

d?

d?

Range

0.0582 - 0.3648 (c)

0.17- 0.33 (c)

0.18-0.34(r)

0.254-0.291 (fe)

0.160-0.550

0.1230-0.3015

Mean

0.2219 ± 0.0698 (c)

0.285 ± 0.020

0.31 ± 0.02 (f)

0.26 ±0.02(f)

0.276 ±0.013

0.270 ± 0.040 (ct)

0.26 ± 0.05 (c)

0.27 ±0.04(0

0.272 ± 0.018 (te)

0.2236 ±0.0190

0.28 ±0.03

0.1830 W, 0.0001

0.22 ± 0.02 (c)

0.20 ± 0.03 (del)

0.17±0.03(c/)

0.246 ±0.035

0.226 ±0.004

0.31

0.369 (op)

Median

0.284

0.270

0.25

0.27

Number of

Samples

30

30 (18 M, 12 F)

45

17 M, 28 F

5

3M.2F

12

8M,4F

12

8M,4F

174

1,M

42

28M.14F

18

11M,7F

7

8

8

22?

3

3

Analytical

Technique

ICPAES

AAS

& ICPAES

EDX

NAA

NAA

&IGAA

PIGE

PIGE

ICPAES

NAA

ICPAES

ICPAES

NAA

NAA

ICPES

ICPAES

ICAP

NAA

48

Reference

Hyvonen-Dabek, 1981

Lindh, 1981

Panday et al., 1980

Bush etal., 1995

Yoshingaetal., 1995

Samudralawar and Robertson, 1993

Hisanaga et al., 1989

Yoshinaga et al., 1989

Kosugi et al., 1988

Zwanziger et al., 1987 & 1985

Mahanti and Barnes, 1983

Niebergall etal., 1983

Niese etal., 1982

HyvSnen-Dabeketal., 1981

Location

Japan

USA

Japan

Japan

Japan

Age

yrs.

24-70

65

18-85

61-96

60-82

40-60

0.17-82

24-70

Sample

Preparation

f

d

d

w

d

d

f

d

d

d

d?

a

d?

d ?

f

Range

0.1580-0.2550

0.06-0.29 (c)

0.32 -1.36

1.5-3.6(n = 6)

Mean

0.260 (pm)

0.309 (of)

0.2078 ±0.029

0.39

0.01

0.031

0.14 ± 0.06 (c)

<3.0

1.2 ± 0.2 (c)

1.01 ± 0.4 (ct)

6.8 ±1.6

<2.5

5.32 x/, 1.9

<1.0

1.56 ±0.08

6.2

7.6 (op)

3.0 (pm)

3-5 (of)

<2.3

Median

<3.0

1.20

1.20

Number of

Samples

15

1M

30

(18M,12F)

45

17M.28F

5

8

11

0

11(7 M.4F)

6

3

3

15

9M.6F

Analytical

Technique

PIGE

PKE

NAA

AAS

AAS

& ICPAES

PKE

AAS

ICPAES

ICPAES

NAA

ICPAES

ICAP

NAA

PKE

49

Reference

Stein et al., 1979

Yoshinga etal., 1995

Lin and Wen, 1988

Jaksic et al., 1987

* < * }

Zaichick, 1994

Samudralawar and Robertson, 1993

Yoshinaga etal., 1989

HyvSnen-Dabek, 1981

Lindh, 1981

Yoshinga etal., 1995

Location

Japan

China

USA

Japan

Japan

Age

yrs.

>10

66

60-82

0.17-82

24-70

65

61-96

Sample

Preparation

d?

d

a

m

d

f

d

f

d

d

Range

< 0.08-0.1

11.4-13.0

Mean

5.7 ±2.2

2.3 ± 0.6

2.8 ±2.1

0.066 ± 0.039 (M)

0.065 ± 0.048 (F)

30 (e)

21 (a)

11 (cm)

5.05 ±0.26

4.8 ± 0.6 (c)

4.4 ± 0.6 (c)

4.92 ±0.18

12.2 ±0.8

4.49

0.518 ±0.046

Median

<0.08

4.6

4.2

0.514

Number of

Samples

35

l l .M

8.F

3

4

4

12

8M,4F

42

28M.14F

15

1M

45

Analytical

Technique

AAS

ICPMS

NAA

PDCE

NAA

&IGAA

PIGE

N

PIGE

PKE

AAS

50

Reference

Zaichick, 1994

Samudralawar and Robertson, 1993

Robertson etal., 1992

Edward, 1990

Yoshinaga et al., 1989

Kosugietal., 1988

Grynpas et al., 1987

Zwanziger et al., 1987 & 1985

Mahanti and Barnes, 1983

Gawlik et al., 1982

Niese etal., 1982

Hyvonen-Dabek, 1981

Lindh, 1981

Pandayetal., 1980

Location

USA.

USA

Japan

Japan

Age

yrs.

60-82

60-82

65

0.17-82

24-70

65

Sample

Preparation

d

f

f

w

d

d

d

d ?

a

d

d?

f

d

d

w

Range

0.350 - 0.640 (c)0.460-0.610(0

0.350-0.740

0.5230-0.6720

Mean

0.638 ± 0.055

0.540 ± 0.060 (ct)

0.520 ±0.080 (c)0.520 ± 0.060 (f)

0.4961 ±0.017

0.523 ±0.988

0.3880 x/, 0.0001

0.3160 x/, 0.00012

0.60 ± 0.03 (c)

0.62 ± 0.09 (del)

0.52 ± 0.14 (ct)

1.066 ±0.02

0.490 ±0.090

1.401 (op)

1.309 (pm)

1.476 (of)

0.5763 ±0.0371

0.58

0.805

0.25

Median

0.520

0.5100.510

0.54

Number of

Samples17 M, 28 F

12

8M.4F

12

8M.4F

l .M

42

28M.14F

11(7M,4F)

7(4M,3F)

7

8

8

3

15

1M

Analytical

Technique&ICPAES

NAA

PIGE

PIGE

NAA

ICPAES

ICPAES

NAA

NAA

ICPAES

NAA

NAA

PIGE

PKE

NAA

51

Reference

Yoshinga et al., 1995

Yoshinga et al., 1995

Baranowska et al., 1995

Yoshinga etal., 1995

Samudralawar and Robertson, 1993

Robertson et al., 1992

Hisanaga et al, 1989

Yoshinaga etal, 1989

Kosugi et al, 1988

Mahanti and Barnes, 1983

Knuuttila etal, 1982

Hyvdnen-Dabek et al, 1981

Location

Japan

Japan

Poland

Japan

USA

USA

Japan

Japan

Japan

Age

yrs.

26-55

61-96

60-82

60-82

40-60

0.17-82

24-70

Sample

Preparation

d

d

f

d

f

f

d

d

d

a

d ?

f

Range

< 0.02-1.0

0.14-2.58

0.14-0.60

< 1.2- 7.8 (c)

< 1.2-4.9(f)

1.9-3.0(n = 4)

Mean

0.38 ±0.55

0.26 ±0.15

<1.5

2.6±2.1(c)

2.3 ± U ( c Q

1.8 ± 2.1 (c)

1.6 ±1.3(0

9.12 ±1.82

0.42 ±0.40

0.32 x/. 1.7

2.1 ±0.02

1.29

<2.4

Median

<0.1

<0.02

1.50

1.40

1.5

1.2

<0.4

Number of

Samples

35

35

25 (15 M, 10 F)

10 (7M, 3 F)

45

17M.28F

10

10

6

7

11

40

18

11M,7F

3

15

9M.6F

Analytical

Technique

ICPMS

ICPMS

AAS

AAS

&ICPAES

PKE

PKE

AAS

ICPAES

ICPAES

ICPAES

AAS

PKE

52

Reference

Samudralawar and Robertson, 1993

Robertson et al., 1992

Hyvdnen-Dabek, 1981

Lindh, 1981

HyvSnen-Dabek, 1979

Yoshinga et al., 1995

Akesson et al., 1994

Zaichick, 1994

Samudralawar and Robertson, 1993

Robertson etal., 1992

Location

USA

USA

Japan

USA

USA

Age

yrs.

60-82

60-82

24-70

65

61-96

40-76

60-82

60-82

Sample

Preparation

f

f

f

d

f

d

d?

d

f

f

Range

6-35(c)

26-38(0

30.4-38.1

4.1- 11.2 (c)6.5-11.1(0

Mean

30 ± 7 (cQ

30 ± 8.2 (c)33 ±3.8(034.8 ± 2.3

40.52

44.8 ± 0.8 (M)

45.0 ± 0.9 (F)

45.6 ± 1.2 (M)

45.1 ± 1.2 (F)

11.9 ±4.0

10.5 ±0.1(0

9.8 ±0.2(0

10.0 ±0.4(0

10.9 ±0.7

9.6 ± 1.3 (cQ

8.8 ± 2.1 (c)9.4 ±1.3(0

Median

33.0

32

33

120

73

9.5

9.8

Number of

Samples

12

8M.4F

12

8M.4F

15

1M

8M

3F

8M

3F

45

17 M, 28 F

5

3M,2F

12

8M.4F

12

8M.4F

Analytical

Technique

PIGE

PIGE

PIGE

PIXE

RBS

AAS

& ICPAES

EDX

NAA

ICPES

NAA

&IGAA

PIGE

PIGE

53

Reference

Katie etal., 1991

Yoshinaga et al., 1989

Kosugi et al., 1988

Giynpas et al., 1987

Jaksic et al., 1987

Mahanti and Bames, 1983

Niebergalletal., 1983

Gawlik etal., 1982

Hyvonen-Dabek, 1981

Lindh, 1981

Eichhom etal., 1980

Hyvonen-Dabek, 1979

Location

Japan

Japan

Age

JTS.

36-77

0.17-82

66

24-70

65

Sample

Preparation

d

d

d

d

m

a

d ?

d

f

d

d ?

f

Range

10.1-12.9 (re)

8.42 -10.5

Mean

11.5 ± 1.0 (te)

12.3 ±0.40

8.02 x/, 0.12

9.7 ± 0.5 (c)

8.7 ±1.1 (del)

7.1±1.4(cQ

29 (ma)

28 (e)

34(5)

54 (a)

50 (cm)

10 (ma)

22 (e)

26 («•)

31 (cm)

13.8 ±0.2

12.5

9.8 ±0.6

20.4 ±1.3

12.19

10.4 ±4.1

16.6 ± 0.5 (M)

17.4 ± 0.8 (F)

17.3 ± 0.5 (M)

17.1 ± 0.9 (F)

Median

Number of

Samples

174

42

28M.14F

18

11M.7F

7

8

8

33

304

4

33

4

4

3

3

15

1M

8M

3 F

8M

3F

Analytical

Technique

ICPAES

ICPAES

ICPAES

NAA

XRF

PKE

ICPAES

ICAP

NAA

PIGE

PKE

NAA

RBS

54

Reference

Baranowska et al., 1995

Bush etal., 1995

Deibeletal., 1995

Yoshingaetal., 1995

Kniewald etal., 1994

Samudralawar and Robertson, 1993

Keinonen, 1992

Robertson etal., 1992

Manea-Krichten et al., 1991

Erkilla etal., 1990

Hu etal , 1990

Morgan etal., 1990

Saltzmanetal., 1990

Location

Poland

USA

Japan

Croatia

USA

Finland

USA

USA

Finland

England

USA

Age

yrs.

26-55

18-85

61-96

60-82

13-64

60-82

67-96

35.5 ±8.9

50-91

20-74

Sample

Preparation

f

d

f

d

f

f

f

d

w

a

w

w

Range

2.90 -204.53

8.90-40.10

0.23-6.45 (c)

1.4-11.5(0

1.3-45 (c)

1.54-11.75

1.06-5.80

1.8-3.7

5.4-45 (c)

< 1.5-11.5(06.73-23.4

4.4-14.3

10-42

Mean

70.66 ±52.58

24.76 ±11.80

2.2 ± 1.5 (c)

5.0 ±3.9(0

12.6 ± 12.9 (c)

6.55 ±2.93

6.85 ±3.41

5.0 ± 3.3 (c/)

12.3 ± 10.9 (c)

4.9 ±3.4(0

12.8 ±6.0

7.18 ±3.65

4.6±11.3(<6)

33.1 ±31.7 (r/u)

26.7 ± 9.7 (c)

24.4 ± 11.1 (t)

7.2 ±10.8

6.70 ± 3.96 (M)

3.17 ± 0.90 (F)

12.46 ± 8.73 (M)

Median

5.55

3.80

9.1

3.8

Number of

Samples

25 (15 M, 10 F)

10(7M,3F)

30

30 (18 M, 12 F)

6

6

7

45

17M,28F

5

12

8M,4F

15

13M,2F

12

8M,4F

6 (2M, 4F)

22

27

15M.12F

59

46M

8F

46M

Analytical

Technique

AAS

AAS

PKE

PKE

AAS

AAS

&ICPAES

V

PKE

M

PKE

MS

InXRF

AAS

InXRF

AAS

55

Reference

Hisanaga et al., 1989

Kowaletal., 1989

Samuels et al., 1989

Yoshinaga et al., 1989

Hisanga et al., 1988

Kosugi et al., 1988

Somervaille et al., 1988

Aalbers et al. 1987

Valkovic et al., 1987

Somervaille et al., 1986

Jaworowski et al., 1985

Location

Japan

Canada

Canada

Japan

Japan

Japan

England

Netherlands

France

Age

yrs.

40-60

55

3 20

0.17-82

40-60

49.3

16-80

2-75

34-89

Sample

Preparation

d

d

a

d

d

d

w

d

m

a

d

Range

18-50

1.94-8.15

1.0-19

11-570 (x)

13-370 (cm)

11- 840 (ci)

22.3 -65.6 (ml)

17.7- 55.6 (m2)

17.2 - 83.0 (tbs)

6.5- 42.5 (tbf)

22.1 -73.5 (ml)

19.9- 56.8 (ml)

15.1- 79.2 (tbs)

10.0- 60.3 (tbf)

5.0-35

Mean

6.96 ± 2.55 (F)

12.55 ± 10.65 (M)

4.54± 2.04 (F)

4.12 ± 2.49 (M)

2.01± 0.72 (F)

4.47 ±1.98

29.8 ± 13

14.77 ±1.30

3.26 ± 2.42

4.47 ±1.98

0.57 x/, 3.1

9.4 (tb)

5.0 ±3.2

16.9 ±10.1

Median

2.88

4.2

Number of

Samples

8F

46 M

8F

46 M

8F

11

25

30

11

18

11M.7F

20

12M,8F

189 (130 M, 70 F)

9

6M.3F

3

3

21

11

3

3

21

11

22?

Analytical

Technique

AAS

AAS

AAS

ICPAES

AAS

ICPAES

InXRF

AAS

XRF

XRF

AAS

AAS

56

Reference

Mahanti and Barnes, 1983

Wielopolski etal., 1983

Liese, 1982

HyvSnen-Dabeketal., 1981

Lindh, 1981

Wittmers et al., 1981

O'Connor et al., 1980

Grandjean et al., 1979

Emslander, 1978

Takizawa etal., 1990

Henshaw et al., 1987

Yoshingaetal., 1995

Location

Sweden

Australia

Denmark

Japan

United Kingdom

Japan

Age

yrs.

24-70

20-77

16-54

45-83

22-82

Sample

Preparation

a

w

d ?

f

a

a

d?

w

w

d

Range

15-35(r)

9.01 • 19.0

10-51

10-34

14-253

1.8 - 7.7

< 0.01-0.3

Mean

22.4 ±0.4

7.7

12.2 ±2.5

14.08 ±1.74

60.85 ± 5.24

47 ±53

5.5

4.9 ±1.5

7.7 ± 2.2

8.78 ± 0.78

Median

<0.01

Number of

Samples

3

15

15

9M,6F

3

3

33

21M.12F

17

9M.8F

20

22

(16M.6F)

4

(2 M, 2 F)

35

Analytical

Technique

ICPAES

AAS

V

PIXE

PKE

AAS

XRF

AAS

AAS

RAD

RAD

ICPMS

57

Reference

Yoshinga et al., 1995

Henshawetal., 1987

Yoshinga et al., 1995

Pietra et al., 1993

Zaichick, 1994

Samudralawar and Robertson, 1993

Robertson et al., 1992

Lin and Wen, 1988

Zwanziger et al., 1987 & 1985

Gawliketal., 1982

Smytheetai., 1982

Location

Japan

United Kingdom

Japan

Italy

USA

USA

China

Australia

Age

yrs.

22-82

60-82

60-82

>10

3 - 80 (80%)

Sample

Preparation

d

w

d

w

d

f

f

a

d ?

d

d

Range

3.29-6.45

< 0.6- 1.8 (c)< 0.6 -2.8(f)

2-62

Mean

1.09 ± 0.38

37.6 ±5.2

2.1 ± 3.0 (c)

2.1 ±3.1 (ct)

1.0 ± 0.5 (c)1.1 ±0.8(0

6.56 ± 3.21 (M)

5.32 ± 3.06 (F)

<0.04

9.5 ±2.8

Median

<0.06

<0.08

1.0

1.0

1.0

1.0

Number of

Samples

35

4

(2 M, 2 F)

35

11

12

9

9

23, M

22, F

7

Analytical

Technique

ICPMS

RAD

ICPMS

NAA

NAA

PDCE

PKE

NAA

NAA

NAA

XRF

58

Reference

O'Connor et al, 1980

Yoshinga et al, 1995

Lindh, 1981

Yoshinga etal, 1995

Zaichick, 1994

Pietra et al, 1993

Zwanziger et al, 1987 & 1985

Zaichick, 1994

Pietra etal, 1993

Location

Australia

Japan

Japan

Italy

Italy

Age

yrs.

20-77

65.

Sample

Preparation

a

d

d

d

d

w

d?

d

w

Range

17-42

< 0.0015-0.00715

0.004-0.081

0.00005-0.0008

Mean

25 ± 7

0.08

0.0151 ±0.0032

0.092 ±0.79

Median

< 0.004

<0.1

Number of

Samples

33

21M,12 F

35

1M

35

Analytical

Technique

XRF

ICPMS

PKE

ICPMS

NAA

NAA

NAA

NAA

NAA

59

Reference

Gawlik et al., 1982

Lin and Wen, 1988

Yoshinga et al., 1995

Zaichick, 1994

Piefra et al., 1993

Mahanti and Barnes, 1983

Gawlik et al., 1982

Smythe et al., 1982

Yoshinga et al., 1995

Yoshinga et al., 1995

Smythe etal., 1982

Location

China

Japan

Italy

Australia

Japan

Japan

Australia

Age

yrs.

>10

3 - 80 (80%)

3 - 80 (80%)

Sample

Preparation

d

a

d

d

w

a

d

d

d

d

d

Range

0.150-0.480

< 0.004-0.2

< 0.21 -7.2

Mean

0.0014 ±0.0007

0.19 ± 0.20 (M)

0.12 ± 0.086 (F)

0.226 ±0.073

0.101 ±0.002

0.13 ±0.4

0.56 ±0.19

2.3 ±0.8

Median

< 2

< 0.004

<0.79

Number of

Samples

23, M

24, F

35

3

2

35

35

7

Analytical

Technique

NAA

NAA

ICPMS

NAA

NAA

ICPAES

NAA

XRF

ICPMS

ICPMS

XRF

60

Reference

Yoshinga et a!., 1995

Kniewald et al., 1994

Zaichick, 1994

Samudralawar and Robertson, 1993

Robertson etal., 1992

Katie etal., 1991

Edward, 1990

Yoshinaga et al., 1989

Kosugi et al, 1988

Lin and Wen, 1988

Jaksic etal, 1987

Location

Japan

Croatia

USA

USA

Japan

Japan

China

Age

yrs.

61-96

60-82

60-82

36-77

65

0.17-82

>10

66

Sample

Preparation

d

f

d

f

f

d

w

d

d

a

m

Range

515.3-592.6

39-97(e)

38 -107 (r)

50 - 72 (te)

Mean

80.5 db 19.6

418±61

58±17(c/)

62 ± 18 (c)

60 ± 18 (t)

67.5 ± 6.8 (te)

90.1 ± 10.3

84.4 ±20.9

48.1 x/, 1.3

213.8 ± 109.4 (M)

251.6 ± 131.4 (F)

105 (ma)

90 (e)

69 (s)

94 (ci)

108 (cm)

65 (ma)

141(e)

258 (ci)

174 (cm)

Median

78.5

55

56

55

83.3

Number of

Samples

45

17 M, 28 F

5

12

8M.4F

12

8M.4F

174

1,M

42

28M,14F

18

11M.7F

23, M

24, F

33

304

4

33

4

4

Analytical

Technique

AAS

&ICPAES

ICPAES

NAA,XRF

&IGAA

PIXE

PKE

ICPAES

NAA

ICPAES

ICPAES

NAA

XRF

PIXE

61

Reference

Zwanziger et a l , 1987 & 1985

Mahanti and Barnes, 1983

Knuuttila et a!., 1982

Gawlik et al, 1982

Nieseetal, 1982

Smythe et al , 1982

Hyv3nen-Dabek et al , 1981

O'Connor etal , 1980

Yoshinga et al, 1995

Lin and Wen, 1988

Yoshinga etal , 1995

Zaichick, 1994

Lin and Wen, 1988

Location

Australia

Australia

Japan

China

Japan

China

Age

.vs.

3 - 80 (80%)

24-70

20-77

>10

>10

Sample

Preparation

d ?

a

d ?

d

d ?

d

f

a

d

a

d

d

a

Range

40-112

26.7-73.0

72-281

< 0.008-0.07

< 0.004-0.02

Mean

149 ±2

65.5

79 ±23

48.8 (op)

71.7 (pm)

48.2(0/)

62 ±27

47.7 ±14.3

121 ±41

0.04 ± 0.020 (M)

0.047 ± 0.037 (F)

0.0344 ±0.0083

0.013 ± 0.034 (M)

Median

< 0.008

< 0.004

Number of

Samples

3

7

15

9M,6F

33

21M.12F

35

15, M

15, F

35

19, M

Analytical

Technique

NAA

ICPAES

AAS

NAA

NAA

XRF

PKE

XRF

ICPMS

NAA

ICPMS

NAA

NAA

62

Reference

Yoshinga et al., 1995

¥»{a<gfe$

Yoshingaetal., 1995

Lin and Wen, 1988

3t<st<g?&g}

Yoshingaetal., 1995

Yoshinagaetal., 1989

Kosugi et al., 1988

Mahanti and Bames, 1983

Yoshingaetal., 1995

Location

Japan

Japan

China

Japan

Japan

Japan

Japan

Age

yrs.

>10

61-96

0.17-82

Sample

Preparation

d

d

a

d

d

d

a

d

Range Mean0.015 ± 0.0056 (F)

0.38 ± 0.23 (M)

0.24 ± 0.094 (F)

<3.0

<5.0

1.95 x/. 1.3

<1.0

0.5 ±0.01

Median

<0.3

<0.06

<3.0

< 0.008

Number of

Samples13, F

35

35

13, M

H , F

45

17 M, 28 F

0

11(7M,4F)

7(4M,3F)

3

35

Analytical

Technique

ICPMS

ICPMS

NAA

AAS

& ICPAES

ICPAES

ICPAES

ICPAES

ICPMS

63

Reference

Yoshinga et al., 1995

tJ{sng%>

Yoshinga et al., 1995

Edward, 1990

Lianqing and Guiyun, 1990

Igarashi et al., 1987

Narayan et al., 1987

Wrennetal.,1985

Fisenne et al., 1984

Fisenne et al., 1983

Fisenne et al., 1983

UNSCEAR, 1982

Fisenne et al., 1980

ICRP, 1979

Location

Japan

Japan

China

Japan

USA

USA

Russia

Australia

Nepal

USA

Age

yrs.

65

21 ->61

37-94

Sample

Preparation

d

d

w

a

w

a

a

a

a

a

a

Range

0.00021-0.00092

0.00033-0.00133

0.00032 - 0.00065

0.002-0.40

0.0009-0.023

0.011

0.0035

0.016

0.022

0.0008

0.022

Mean

<0.5

0.061-0.062

0.00067 ±0.00026

0.00083 ±0.00036

0.00055 ±0.00019

Median

< 0.004

< 0.004

Number of

Samples

35

35

1,M

30

15M.15F

6

3M.3F

7

4M.3F

7(4M,3F)

5

8

9

Analytical

Technique

ICPMS

ICPMS

NAA

LF

FT

FT

FT

AAS

AAS

AAS

R

64

Reference

Yoshinga etal., 1995

Yoshinaga et al, 1989

Kosugi etal., 1988

Mahanti and Barnes, 1983

Yoshinga et al., 1995

Pietra et al , 1993

Yoshinga et al, 1995

Yoshinga et al, 1995

Location

Japan

Japan

Japan

Japan

Italy

Japan

Japan

Age

yrs.

61-96

0.17-82

Sample

Preparation

d

d

d

a

d

w

d

d

Range

< 0.08-1.2

0.0007-0.00275

< 0.03-0.3

< 0.004 -0.02

Mean

<6.0

<5.0

4.09 x/, 1.3

<2.0

1.1 ±0.03

Median

<6.0

<0.08

<0.03

< 0.004

Number of

Samples

45

17M.28F

0

11(7 M.4F)

7(4M,3F)

3

35

35

35

Analytical

Technique

AAS

& ICPAES

ICPAES

ICPAES

ICPAES

ICPMS

NAA

ICPMS

ICPMS

65

Reference

Baranowska et al., 1995

Bush etal., 1995

Yoshinga et al., 1995

Kniewald et a!., 1994

Pietraetal., 1993

Zaichick, 1994

Samudralawar and Robertson, 1993

Robertson etal., 1992

Katie etal., 1991

Saltzman et al., 1990

Yoshinagaetal., 1989

Kosugi et al., 1988

Location

Poland

Japan

Croatia

Italy

USA

USA

USA

Japan

Japan

Age

yrs.

26-55

18-85

61-96

60-82

60-82

36-77

20-74

0.17-82

Sample

Preparation

f

d

d

fw

d

f

f

d

w

d

d

Range

85.7-138.3

86.4 -138.8

71-157 (c)

33-88

40.5-63

115-293(c)

117-181(f)

258-282 (fe)

Mean

118.22 ± 12.96

107.41 ± 15.22

114± 18.1 (c)

149 ±19

91.0 ±4.4

144±17(e/)

182±47(e)

144 ±18(0

265.8 ± 15.4 (te)

42.01±9.11(M)

46.79 ± 4.70 (F)

54.26 ± 12.28 (M)

57.87 ± 11.03 (F)

38.62 ± 8.59 (M)

33.71 ± 4.25 (F)

25.96 ± 6.52 (M)

29.83 ± 2.79 (F)

139 ±25

120 x/, 1.2

Median

142

139

179

139

134

Number of

Samples

25 (15 M, 10 F)

10(7M,3F)

30

30 (18 M, 12 F)

45

17 M, 28 F

5

12

8M.4F

12

8M,4F

174

21 M

5 F

21 M

5F

21 M

5F

21 M

5F

42

28M.14F18

Analytical

Technique

AAS

ICPAES

AAS

& ICPAES

V

NAA

NAA

&XRF

PKE

PKE

ICPAES

AAS

ICPAES

ICPAES

66

Reference

Lin and Wen, 1988

Jaksic et al., 1987

Valkovicetal., 1987

Zwanzigeretal., 1987 & 1985

Jaworowski et al., 1985

Mahanti and Barnes, 1983

Lappalainen et al., 1982

Gawliketal., 1582

Sraythe et al., 1982

Hyvonen-Dabeketal., 1981

Lindh, 1981

O'Connor etal., 1980

Location

China

France

Australia

Sweden

Australia

Age

yrs.

>10

66

2-75

34-89

3 - 80 (80%)

24-70

20-77

Sample

Preparation

a

m

m

d?

d

a

d ?

d

d

f

a

Range

53 - 855 (s)

195 -1010 (cm)

100 -1060 (ci)

59-244

78 -170

96.9 -181

38-186

30-129

174-299

Mean

178.8 ± 97.2 (M)

148.9 ± 82.8 (F)

187 (ma)

255 (e)

221 (s)

325 (ci)

343 (cm)

407 (ma)

353 (e)

429 (ci)

426 (cm)

126 ±21

102.0 ±1

113.9 ±40.7

151 ±22

98 ±16

144 ±27

221 ±30

Median

Number of

Samples11M,7F

23, M

24, F

33

304

4

33

4

4

10

7M,3F

22?

3

13887M,51F

7

15

9M.6F

3

3

33

21M,12F

Analytical

Technique

NAA

XRF

PKE

XRF

NAA

ICPES

ICPAES

AAS

NAA

XRF

PKE

PKE

XRF

67

Reference

Yoshingaetal., 1995

Lin and Wen, 1988

Location

Japan

China

Age

yrs.

>10

Sample

Preparation

d

a

Range

< 0.3-0.4

Mean

44.30 ± 46.63 (M)

42.69 ± 29.92 (F)

Median

<0.3

Number of

Samples

35

15, M

13, F

Analytical

Technique

ICPMS

NAA

68

TableNotations used in Teeth Compilation

a = ashed

d = dry weight basis

f= freeze dried

m = macerated

n = no sample preparation

e — enamel

se = surface enamel

d = dentine

cd = coronal dentine

id = inner dentine

od - outer dentine

sd = surface dentine

c = cementum

p =pulped

cpd = circumpulpal (or secondary) dentine

pd = pulpal dentine

pf=pulp free

AAS = atomic absorption spectrometryC = colorimetry

CPAA = charged particle activation analysis

FT = fission track methodIGAA = instrumental gamma-activation analysisICPAES = inductively-coupled plasma atomic emission spectrometryICPMS = inductively-coupled plasma mass spectrometryISE = ion-selective electrodeMS = mass spectrometry

NAA = neutron activation analysis

PIXE = proton induced x-ray emissionPIGE = proton induced gamma-ray emissionPGAA = prompt-gamma activation analysisXRF = x-ray fluorescenceV = voltametry

ICS = in-house calibration standard

L = no QA/QC mentioned but agreement with the literature values

* not clear

f* = Fergusson and Purchase, 1986 (Review article), not clear

B* = Bercovitz et al, 1993, not clear.

69

Table 4 A:Major, Minor and Trace Elemeiit in Human Teeth

(The references include onlv permanent teeth i.e. no deciduous teeth)

Reference

Johansson, 1991

Cutress, 1979

Curzon and Crocker, 1978

Curzon and Losee, 1978

Vrbic et al., 1987

Cutress, 1979

Curzon and Crocker, 1978

Lindh and Tveit, 1980

Ward, 1987

Cutress, 1979

Curzon and Crocker, 1978

Curzon and Losee, 1978

Location

14 Countries

Area

USA & New Zealand

USA

Yugoslavia

14 Countries

Oregon

California

Dalmatia

USA & New Zealand

New Zealand

14 Countries

USA & New Zealand

USA Oregon

California

Age

yrs

10-20

<20

<20

38-61

10-20

69-84

10-20

<20

<20

Sample

Prep

*

d

n

d

d

d

Range

0.2- 396 (se)

0.0-36.6 (e)

16- 2304 (se)

0.0- 510.0 (e)

0.8 - 13.0 (se)

0.0-190.0 (e)

Mean

0.08

32 (se)

3.44 (e)

0.26 ± 0.07 (e)

0.06 ± 0.01 (e)

2.1 ± 1.08 (e)

343 (se)

22.89 (e)

<14(e)

4.12 ±1.13

5.3 (se)

8.40 (e)

5.79 ± 1.87 (e)

0.87 ± 0.16 (e)

Median

Z(se)

202 (se)

3.6 (se)

#of

Samples

4

54

244

41

42

20

54

335

1M

(20 spots)

14

54

337

40

42

Analytical

Technique

ICPMS

MS

MS

MS

AAS

MS

MS

PKE

PGAA

MS

MS

MS

70

Reference

Manea-Krichtenetal., 1991

Vrbicetal., 1987

Cutress, 1979

Curzon and Crocker, 1978

Curzon and Losee, 1978

Cutress, 1979

Cutress ,1979

Curzon and Crocker, 1978

M611er and Carlsson, 1984

Cutress, 1979

Curzon and Crocker, 1978

Nowak, 1995

Manea-Krichten et al., 1991

Knuuttila et al., 1985

Location

USA

Yugoslavia

14 Countries

Area

Dalmatia

USA & New Zealand

USA

14 Countries

14 Countries

Oregon

California

USA & New Zealand

Sweden

USA

14 Countries

New York City

USA & New Zealand

Poland

USA

Urban (Industrial)

Rural

Age

yrs

67-96

38-61

10-20

<20

<20

10-20

Children

10-20

11-60

67-96

10-74

Sample

Prep

d

n

d

d

d

d

d

d

d

d

Range

2.83 -15.7 (e)

0.8-432 (se)

0.0-510.0 (e)

0 - 0.04 (se)

0-6.1(se)

0.0-15.9 (e)

1.43±1.29-1.50±1.23(cd)

0.57±0.96-1.23±0.59(c<f)

0.4-14.0 (se)

0.0-33.2 (e)

35.2-37.3 (e)

Mean

6.4 (e)

7.7 ± 1.8 (e)

22 (se)

18.83 (e)

5.13 ± 1.18 (e)

2.02 ± 0.69 (e)

0.001 (se)

1.3 (se)

1.36 (e)

3.1 (se)

4.54 (e)

9.97 ±1.55

11.7 ±1.6

36.5 (e)

35.5 ± 4.3 (e)

Median

7(se)

0(se)

1.2 (se)

4.1 (se)

#of

Samples

6 (2M, 4F)

20

54

334

40

42

3

25

241

11

12

54

287

62

102

6 (2M, 4F)

40

Analytical

Technique

MS

AAS

MS

MS

MS

MS

MS

MS

PKE

MS

MS

AAS

MS

AAS

71

Reference

Cohen etal., 1981

Lindh, 1981

LindhandTveit, 1980

Nowak, 1995

Cleymaet et al., 1991

Grandjean and Jorgensen, 1990

Vrbic etal., 1987

Lappalainen and Knuuttila, 1979

Cutress, 1979

Curzon and Crocker, 1978

Curzon and Losee, 1978

Oehme etal., 1978

Cohen etal., 1981

Lindh, 1981

Location

Australia

Poland

Belgium

Kenya

Greenland

Denmark

Yugoslavia

Finland

14 Countries

Area

Urban (Industrial)

Rural

Urban (Industrial)

Rural

Ummannaq-Nuuk

Funen

Dalmatia

5 Areas

USA & New Zealand

USA

Norway

Australia

Oregon

California

Urban

Age

vrs

65

11-60

6-12

10-43

10-62

38-61

10-72

10-20

<20

<20

Teens

65

Sample

Prep

d

d

d

d

*

d

n

d

d

d

d

d

Range

36.6-37.1(e)

0.042- 0.363 (cpd)

0.035- 0.314 (cpd)

2.7-6.3

0.6- 7.6 (se)

0.0-27.0 (e)

< 0.04-16.2

1600- 2800 (e)

2500- 2600 (d)

Mean

31.5 ±2.1 (e)

31.5 ±1.1 (d)

37.34 (e)

36.9 (e)

2.2 ±0.89

1.7 ±0.77

9.1 ± 8.02 (se)

6.4 ±3.8 (re)

0.03 ± 0.02 (e)

4.2 ±0.7

2.7 (se)

1.87 (e)

1.56 ± 0.32 (e)

0.31 ± 0.06 (e)

7900 (e)

Median

7.1

5.4

0.086 (cpd)

0.097 (cpd)

1.8 (se)

#of

Samples

24M,16F

15

1M

1M

(20 spots)

62

102

249

60

14

7M.7F

33

28M.5F

20

124 .

54

334

40

42

10

15

1M

Analytical

Technique

PKE

PKE

PKE

AAS

AAS

AAS

AAS

AAS

MS

MS

MS

V

PKE

PKE

72

Reference

Lindh and Tveit, 1980

Cutress, 1979

Nowak, 1995

Ngwenya and Turkstra, 1985

Lappalainen and Knuuttila, 1982

Lindh and Tveit, 1980

Lappalainen and Knuuttila, 1979

Cutress, 1979

Curzon and Crocker, 1978

Nowak, 1995

Ngwenya and Turkstra, 1985

Location

14 Countries

Poland

South Africa

Finland

Finland

14 Countries

Area

Urban (Industrial)

Rural

3 Areas

*3 Ethnic groups

5 Areas

USA & New Zealand

Poland

South Africa

Urban (Industrial)

Rural

3 Areas

*3 Ethnic groups

Age

yrs

11-60

10-76

10-72

10-20

11-60

Sample

Prep*

d

d

d

d

d

d

d

d

d

d

d

Range

8600 - 9300 (e)

0-6.1 (a;)

0.41 - 2.69 {d)

0.12-1.61 (e)

0.0- 0.3 (d)

18.3-34.8

0-2.7(se)

0.0 -1.5 (e)

0.83 -3.28(rf)

1.00- 3.90 (d)

0.07-0.45 (e)

0.13-0.62 (e)

Mean

8900 (e)

0.6 (se)

6.51 ± 1.75

4.8 ± 2.42

0.1 ±0.1 (d)

<16(e)

24.8 ±3.0

0.2 (se)

0.27 (e)

47.2 ± 7.87

42.6 ± 6.79

Median

0(se)

0.1 (se)

#of

Samples

1M

(20 spots)

23

62

102

123

72M,51F

1M

(20 spots)

124

47

246

62

102

Analytical

Technique

PKE

MS

AAS

AAS

AAS

PKE

AAS

MS

MS

AAS

AAS

COL

AAS

COL

73

Reference

Cohen etal., 1981

Coles etal., 1980

Lindh and Tveit, 1980

Cutress, 1979

Curzon and Crocker, 1978

Cutress, 1979

Nowak, 1995

Vrbic etal., 1987

Ngwenya and Turkstra, 1985

Moller and Carlsson, 1984

Lappalainen and Knuuttila, 1982

Cohen etal., 1981

Lindh and Tveit, 1980

Location

Australia

England

14 Countries

Area

USA & New Zealand

14 Countries

Poland

Yugoslavia

South Africa

Sweden

USA

Finland

Australia

Urban (Industrial)

Rural

Dalmatia

3 Areas

*3 Ethnic groups

New York City

Age

yrs

10-20

11-60

38-61

Children

10-76

Sample

Prep

d

d

d

d

d

d

n

d

d

d

Range20-40(e)

15-30(tf)

0.2-4.7(5e)

0.0-18.0 (e)

0 -1.9 (se)

0.09 -1.20 (d)

0.64- 2.75 (d)

0.14-0.84 (e)

0.07-1.00 (e)

0.79±1.35 -1.30±1.03 (cd)

3.77±13.05 - 5.11±13.30 (cd)

0.5-11.8 (d)

10-30(e)

15 - 50 (d)

10 - 26 (e)

Mean

<34(e)

1.1 (M)

0.45 (e)

0.1 (se)

• 9.74 ±30.6

6.8 ±25.25

0.92 ± 0.76 (e)

3.0 ± 2.0 (d)

21 («)

Median

0.4

0.7 (se)

0(se)

#of

Samples

15

37?

1M

(20 spots)

54

236

23

62

102

20

11

12

123

72M.51F

15

1M

(20 spots)

Analytical

Technique

PKE

AAS

PKE

MS

MS

MS

AAS

AAS

AAS

COL

AAS

COL

PKE

AAS

PDflE

PKE

74

Reference

Lappalainen and Knuuttila, 1979

Cutress, 1979

Curzon and Crocker, 1978

Curzon and Losee, 1978

Oehme et al., 1978

Knuuttila et al., 1985

Cutress, 1979

Curzon and Crocker, 1978

Curzon and Losee, 1978

Nowak, 1995

MdllerandCarlsson, 1984

Location

Finland

14 Countries

Area

5 Areas

USA & New Zealand

USA

Norway

14 Countries

Oregon

California

Urban

USA & New Zealand

USA

Poland

Sweden

USA

Chaudhari and Crawford, 1981

Cohen etal, 1981

Lindh and Tveit, 1980

Cutress, 1979

Curzon and Crocker, 1978

Australia

14 Countries

Oregon

California

Urban (Industrial)

Rural

New York City

USA & New Zealand

Age

yrs

10-72

10-20

<20

<20

Teens

10-74

10-20

<20

<20

11-60

Children

10-20

Sample

Prep

d

d

d

d

d

d

d

d

*

d

Range

7.5-22.7

13 -1260 (se)

0.0 - 30 (e)

1.3 -16.8

25 - 1948 (se)

8.6 - 925.0 (e)

2.52±2.82 - 3.06±2.36 (cd)

6.12±8.66-7.02±8.02(<aQ

15 -100 (e)

15-30(<0

25 -142 (e)

18- 1404 (se)

0.0-157.0 (e)

Mean

9.76 ± 2.88

282 (se)

1.50 (e)

0.21 ± 0.04 (e)

0.68 ± 0.15 (e)

110±40(e)

752 (se)

130.27 (e)

54.3 (e)

55 (e)

32.03 ±12.11

34.4 ±16.01

65

85 (e)

138 (se)

27.95 (e)

Median

241 (se)

666 (se)

68 (se)

#of

Samples

124

54

336

40

41

10

40

24M,16F

54

337

62

102

11

12

15

1M

(20 spots)

54

337

Analytical

Technique

AAS

MS

MS

MS

V

ISE

MS

MS

MS

AAS

PKE

PKE

PKE

MS

MS

75

Reference

Cutress, 1979

Cutress, 1979

«£#ftga#

Johansson, 1991

Lindh and Tveit, 1980

Cutress, 1979

Curzon and Crocker, 1978

Nowak, 1995

Lindh and Tveit, 1980

Curzon and Crocker, 1978

Curzon and Losee, 1978

La£tt>g&g)

Cutress, 1979

Location

14 Countries

14 Countries

14 Countries

Area

USA & New Zealand

Poland Urban (Industrial)

Rural

USA & New Zealand

USA

14 Countries

Oregon

California

Age

yrs

10-20

11-60

10-20

<20

<20

Sample

Prep

d

d

*

*

d

d

d

*

d

Range

0-32(«0

0.5- 39.6 (se)

0-4.7 (.ye)

0.0-9.9 (e)

900 -1600 (e)

59.6- 4056.0 (e)

0-7.2(se)

Mean

6(se)

7.6 (se)

0.2

<22(e)

0.05 (se)

2.04 (e)

53.47 ±13.45

53.3 ± 8.36

1200 (e)

961.41 (e)

333.95 ± 42.61 (e)

191.04 ± 30.33 (e)

1.4 (se)

Median

5(se)

4(se)

0.05 (se)

0.8(se)

# of

Samples

29

54

4

1M

(20 spots)

26

92

62

102

1M

(20 spots)

337

40

42

51

Analytical

Technique

MS

MS

ICPMS

PKE

MS

MS

AAS

PKE

MS

MS

MS

76

Reference

Vrbic etal., 1987

Cutress, 1979

Curzon and Crocker, 1978

Knuuttilaetal., 1985

Lappalainen and Knuuttila, 1982

Cohen etal., 1981

Lindh, 1981

Cutress, 1979

MiU-rog&g)

Nowak, 1995

Ngwenya and Turkstra, 1985

Lappalainen and Knuuttila, 1982

Cohen etal., 1981

Lindh and Tveit, 1980

Location

Yugoslavia

14 Countries

Area

Dalmatia

USA & New Zealand

Finland

Australia

14 Countries

Poland

South Africa

Finland

Australia

Urban (Industrial)

Rural

3 Areas

*3 Ethnic groups

Age

yrs

38-61

10-20

10-74

10-76

65

11-60

10-76

Sample

Prep

n

d

d

d

d

d

d

d

d

d

d

d

Range

0.3 -58 (se)

0.0-13.2 (e)

5400-11100 (d)

1000-1100 (e)

3000-8000(0

115-3600(re)

0.98- 2.96 (d)

1.58- 3.00 (d)

0.20-1.62 (e)

0.09-2.02 (e)

0.4-17.1 (d)

5-25<«)

5 - 20 (d)

Mean

0.53 ± 0.14 (e)

14 (se)

0.92 (e)

2400 ± 500 (e)

7926 ± 1044 (d)

4100 (e)

745 (se)

47.65 ± 16.93

39.3 ± 10.2

3.9 ±2.5 (d)

<25(e)

Median

10 (se)

576 (se)

#of

Samples

20

54

246

40

24 M, 16 F

123(72M, 51F)15

1M

54

62

102

123

72M.51F

15

1M

Analytical

Technique

AAS

MS

MS

AAS

AAS

PKE

PKE

MS

AAS

AAS

COL

AAS

COL

AAS

PKE

PKE

77

Reference

Lappaiainen and Knuuttila, 1979

Cutress, 1979

Curzon and Crocker, 1978

Jasimetal., 1988

Vrbicetal., 1987

Cutress, 1979

Curzon and Crocker, 1978

Lindh, 1981

Nowak, 1995

Cohen et al , 1981

Lindh, 1981

Curzon and Crocker, 1978

Nowak, 1995

Location

Finland

14 Countries

Area

5 Areas

USA & New Zealand

Iraq

Yugoslavia

14 Countries

Baghdad

Dalmatia

USA & New Zealand

Poland

Australia

Urban (Industrial)

Rural

USA & New Zealand

Poland Urban (Industrial)

Rural

Age

yrs

10-72

10-20

15-60

38-61

10-20

65

11-60

65

10-20

11-60

Sample

Prep

d

d

d

n

d

d

d

d

d

d

d

Range

5.2-28.9

2.6-468 (.se)

0.0-6.7 (e)

3.2-8.2 (p/)

6.8-9.2 (p)

0.04- 0.5 (se)

0.0- 32.0 (e)

1700-2600 (e)

2000- 2300 (d)

0.0-1.0 (e)

Mean

9.06 ±3.43

59(«)

0.60 (e)

0.84 ± 0.38 (e)

0.1 (se)

2.37 (e)

0.14 (e)

1125.96 ±74.98

1192.8 ±169.73

13600 (e)

0.17(e)

8.42 ±1.35

4.6 ±1.32

Median

33 (se)

0.04 (se)

Hot

Samples

(20 spots)

124

54

336

5

5

20

54

334

1M

62

102

15 -

1M

245

62

102

Analytical

Technique

AAS

MS

MS

AAS

AAS

MS

MS

PKE

AAS

PKE

PKE

MS

AAS

78

Reference

Lappalainen and Knuuttila, 1982

Cohen etal., 1981

Lindh and Tveit, 1980

Lappalainen and Knuuttila, 1979

Cutress, 1979

Curzon and Crocker, 1978

Curzon and Losee, 1978

Knuuttila et al., 1985

Cohen etal., 1981

Lindh, 1981

Lindh and Tveit, 1980

Nowak, 1995

Gil etal., 1994

Bercovitz et al., 1993

Bercovitz and Laufer, 1993

Location

Finland

Australia

Finland

14 Countries

Area

5 Areas

USA & New Zealand

USA

Australia

Poland

Spain

Israel

Israel

Oregon

California

Urban (Industrial)

Rural

Urban & Rural

5 Regions

Northern Region

Age

yrs

10-76

10-72

10-20

<20

<20

10-74

65

11-60

20->60

14-75

Sample

Prep

d

d

d

d

d

d

d

d

d

d

d

d

Range

0.4-1.7 (d)

5-15(<2)

5 - 50 (d)

23.1-44.8

0.4- 270 (se)

0.0-9.0 (e)

19.9-21.5 (e)

0.13-80.37

0.58-36.89

1.24-32.72 (d)

Mean

0.9 ± 0.7 (d)

<13(e)

31.3 ±4.4

23 (se)

0.90 (e)

0.29 ± 0.09 (e)

1.16 ± 0.19 (e)

16.5 ± 1.4 (e)

16.1 ±1.5 (e)

14.0 ±1.8 (d)

17.38 (e)

21 («)

47.65 ± 16.93

39.3 ± 10.2

6.15 x/- 1.21

1.65-25.72

10.95 ±9.11 id)

Median

9(se)

#of

Samples

123

72M,51F

15

1M

(20 spots)

124

54

249

38

40

40

24 M, 16 F

15

1M

1M

(20 spots)

62

102

40

180

22

Analytical

Technique

AAS

PKE

PKE

AAS

MS

MS

MS

C

PDCE

PKE

PKE

AAS

AAS

AAS

AAS

79

Reference

Bercovitz and Laufer, 1991

Cleymaetetal., 1991

Manea-Krichtenetal., 1991

Frank etal., 1990

Grandjean and Jorgensen, 1990

Khadekar et al., 1986

Purchase and Fergusson 1986

Grobleretal., 1985

Kollmeier etal., 1984

Ogawa, 1983

Lappalainen and Knuuttila, 1982

Cohen etal., 1981

Steenhout and Pourtois, 1981

Location

Israel

Belgium

Kenya

USA

Mexico

France

Greenland

Denmark

India

New Zealand

South Africa

Germany

Japan

Finland

Australia

Belgium

Area

Northern Region

Urban (Industrial)

Rural

Urban

Strasbourg

Ummannaq-Nuuk

Funen

Bombay

Urban

Urban & Rural

Urban

Industrial

Age

yrs

31-75

6-12

67-96

12-29

32-65

10-43

10-62

6-1210-70

10-76

Sample

Prepd

*

d

d

d

d

?

d

d

d

d

d

d

a

Range2.11 - 117.37(rf)

4.1-29.8 (e)

5.0 -172 (cpd)

3.5 -163 {cpd)

2.0-28.0

14.3- 29.6 (e)

26.5-74.5

1-30

1.0-39.0(rf)

< 10 (e)

10-30(rf)

5.4-110.7

Mean

25.62± 10.15(41

1236 ± 849 (se)

145±67(se)

14 (e)

24.1 ± 9.3 (od)

118.8 ± 95.6 (id)

45.3 ± 15.8 (id)

8.31x/, 1.20

99 (sd)

20.4 (d)

7.9 (e)

1100(«!)

14.8 (d)

1.55(0

1.7 (e)

13.7 ±8 .5 (0

33.35

Median

1066

134

16.8 (cpd)

23.7 (cpd)

#of

Samples

12

252

60

6 (2M, 4F)

14

7M,7F

33

28M.5F

71

30, M, 41 F

5

8

8

13

171

17

163

123

72M,51F

15

51

Analytical

Technique

AAS

AAS

MS

AAS

V

AAS

AAS

AAS

AAS

PKE

AAS

80

Reference

Al-Naimietal., 1980

Coles et al., 1980

Lindh and Tveit, 1980

Cutress, 1979

Grandjeanetal., 1979

Lappalainen and Knuuttila, 1979

Curzon and Crocker, 1978

Oehmeetal., 1978

Location

Belgium

Belgium

England

England

14 Countries

Denmark

Finland

Area

Rural

Urban

Birmingham

Sheffield

Aberystwyth

Copenhagen

5 Areas

USA & New Zealand

Norway Urban

Age

yrs

12-16

40-7112-16

40-71

12-16

40-71

12-16

40-72

12-16

40-72

12-16

40-72

5-15

40-70

5-15

40-70

5-15

16-54

10-72

10-20

Teens

Sample

Prep

d

d

d

n

d

d

Range

1.2-69.3

2.3-68.0

17.3- 43.9 (pd)

21.0-213.1 (pd)

5.8 -12.6 (d)

5.0- 39.6 (d)

1.6-3.6 (e)

1.4-5.3 (e)

12.5-24.5 (pd)

28.2 - 299.6 (pd)

3.8-10.4 (d)

5.5 - 66.7 (d)

1.4-3.5 (e)

1.2-5.4 (e)

20.8-54.3 (pd)

112.6-310.3 (pd)

4.2-11.1 (d)

26.9 - 81.0 (d)

1.6-2.9 (e)

2.0 - 5.0

1.2-79(«0

30-79.2

0.0 -156.0 (e)

1.8-4.9

Mean

21.45

17.72

34.2 ± 17.0 (pd)

92.2 ±31.9 (pd)

7.2 ± 3.4 (d)

17.3 ± 7.3 (d)

2.3 ± 1.0 (e)

2.7 ± 0.7 (e)

18.9 ± 7.4 (pd)

112.5 ± 52.9 (pd)

7.2 ± 2.9 (d)

25.6 ± 12.4 (d)

2.1 ± 1.0 (e)

4.0 ± 0.7 (e)

27.5 ± 9.6 (pd)

149.3 ± 92.5 (pd)

5.6 ± 2.0 (d)

40.6 ± 22.8 (d)

2.0 ± 0.6 (e)

<21(e)

24 (ye)

25.7 (cpd)

53.5 ± 7.8

19.64 (e)

Median

3.8

18 (se)

#of

Samples

38

42

10

19

10

19

10

19

5

11

5

11

5

11

10

5

10

5

10

37

1M

(20 spots)

54

17

9M.8F

124

335

10

Analytical

Technique

CPAA

AAS

PKE

MS

V

AAS

MS

V

81

Reference

Pinchinetal., 1978

Khandekaretal., 1978

Attramadal and Jonsen, 1976

Wilkinson and Palmer, 1975

Shapiro et al., 1975

Kaneko et al., 1974

Malik and Fremlin, 1974

Stack etal, 1974

Langmyhr et al., 1974

Strehlow and Kneip, 1969

Cutress, 1979

Cutress, 1979

Curzon and Crocker, 1978

Curzon and Losee, 1978

Cohen etal., 1981

Lindh, 1981

Location

England

India

Norway

USA

USA

Japan

England

Scotland

Sweden

USA

14 Countries

14 Countries

Area

Urban

Urban

Urban

Mixed

Rural

Urban

Non-industrial

4 Areas

Urban

Rural

USA & New Zealand

USA

Australia

Oregon

California

Age

yrs

Teens

0-79

0-79

6-59

19-57

Teens

62

< 10-60

10-20

<20

<20

65

Sample

Prep

d

d

d

d

d

d

d

d

d

d

d

a

a

d

d

d

d

Range

1.22-3.60

4.27-82.5

0.9-7.8

H-55

14-67

0-38

1-30

1.12-64.67

25 - 52.7

17-20

1.1-6.4

254-336

17-16

0 - 4.7 (se)

0.1 -4.0 (se)

0.0- 30.0 (e)

1000 -1350 (<?)

700 (d)

Mean

0.2 (se)

0.6 (se)

4.61 (e)

0.33 ± 0.07 (e)

0.15 ± 0.02 (e)

300 (e)

Median

0(se)

0.4 (se)

#of

Samples

8

72

44

336

230

62

163

93

10

36

14

4

14

54

256

32

33

15

1M

Analytical

Technique

V

AAS

V

AAS

AAS

AAS

CPAA

AAS

AAS

AAS

MS

MS

MS

MS

PKE

PDCE

82

Reference

Lindh and Tveit, 1980

Cutress, 1979

Curzon and Crocker, 1978

Cutress, 1979

Curzon and Crocker, 1978

Curzon and Losee, 1978

Ngwenya and Turkstra, 1985

Cutress, 1979

Curzon and Crocker, 1978

Cutress, 1979

Sn(tag/feg)

Lindh and Tveit, 1980

Cutress, 1979

Curzon and Crocker, 1978

Location

14 Countries

Area

USA & New Zealand

14 Countries

USA & New Zealand

USA

South Africa

14 Countries

Oregon

California

3 Areas

*3 Ethnic groups

USA & New Zealand

14 Countries

14 Countries

USA & New Zealand

Age

yrs

10-20

10-20

<20

<20

10-20

10-20

Sample

Prep*

d

d

d

d

d

d

d

Range

812-819 (e)

1836- 40320 (se)

0.0 - 200.0 (e)

0-90(«!)

0.0-3.0 (e)

0.27 -1.03 (d)

0.06-1.03 (e)

2.9-72(se)

0.0 -18.1 (e)

1.3- 504 (se)

0.9-72(«0

0.0- 44.0 (e)

Mean

815 (e)

18780 (se)

24.19 (e)

8(«)

0.20 (e)

0.07 ± 0.0 l(e)

0.02 ± 0.00 (e)

18 (se)

1.47 (e)

70 (se)

<325(e)

9.3 (se)

1.60 (e)

Median

17280 (se)

3(se)

16 (se)

40 (se)

5.8 (se)

#of

Samples

1M

(20 spots)

54

336

26

225

36

41

54

326

54

1M

(20 spots)

54

245

Analytical

Technique

PKE

MS

MS

MS

MS

MS

F-

MS

MS

MS

PKE

MS

MS

83

Reference

Frank etal., 1989

Vrbicetal., 1987

Mdller and Carlsson, 1984

Curzon and Cutress,1983

Curzon.1983

Lappalainen and Knuuttila, 1982

Location

France

Yugoslavia

Sweden

USA

Finland

Chaudhari and Crawford, 1981

Cohen etal., 1981

Lindh and Tveit, 1980

Cutress, 1979

Curzon and Crocker, 1978

Curzon and Losee, 1978

Australia

14 Countries

Area

Strasbourg

Dalmatia

New York City

USA & New Zealand

USA Oregon

Age

yrs

10-27

32-65

38-61

Children

10-76

10-20

<20

Sample

Prep

n

n

d

d

*

d

Range

32.2- 205.0 (cd)

23.5-251.0 (erf)

70-286 (e)

32.5 -138.0 (d)

100-150 (e)

110-150 0 )

96 -108 (e)

9-7632(se)

13.0 -1400.0 (e)

Mean

150.5 ± 55.6 (se)

155.0 ± 51.4 (ie)

94.6 ±43.6 (peed)

92.6 ± 35.6 (med)

87.2 ± 34.7 (ped)

82.9 ± 32.0 (perd)

77.7 ± 30.1 (prd)

196.9 ± 62.3 (se)

206.4 ± 76.2 (ie)

136.7 ± 60.2 (peed)

124.3 ± 41.6 (med)

125.0 ±37.6 (pa/)

123.2 ±46.9 (perd)

132.8 ± 57.3 (prd)

106.7 ± 23.1 (e)

83.3 ± 52.1 (cd)

75.0 ± 59.9 (cd)

80.7 ± 24.3 (d)

23

103 (e)

204 (se)

157.15 (e)

81.51 ± 9.04 (e)

Median

115 (e)

150 (d)

36 (se)

#of

Samples

8

7

20

11

12

123(72M, 51F)

15

1 M (20 spots)

54

337

33

Analytical

Technique

XRF

AAS

PKE

AAS

PKE

PKE

MS

MS

MS

84

Reference

Cutress, 1979

Curzon and Crocker, 1978

Vrbicetal., 1987

Cohen etal., 1981

Byrne and Vrbic, 1979

Cutress, 1979

Curzon and Crocker, 1978

Cutress, 1979

Lindh and Tveit, 1980

Nowak, 1995

Knuuttila etal., 1985

Location

14 Countries

Area

California

USA & New Zealand

Yugoslavia

Australia

Yugoslavia

14 Countries

Dalmatia

Zemunik

Novigrad

Ljubljana

Belgrade

USA & New Zealand

14 Countries

Poland Urban (Industrial)

Rural

Age

yrs

<20

10-20

38-61

10-20

11-60

10-74

Sample

Prep

d

n

d

d

d

*

d

d

d

Range

0.1- 24.5 (se)

0.0-31.4(e)

10-30(e)

15-35(<0

0.1- 14.4 (se)

0.0-0.2 (e)

0-9.3 (re)

Mean

130.51 ± 12.27 (e)

1.6 (se)

1.93 (e)

0.0039 ± 0.0022 (e)

0.0038 ± 0.0013 (e)

0.0041 ± 0.0022 (e)

0.0031 ± 0.0012 (e)

0.0033 ± 0.00 l l ( e )

1.4 (se)

0.02 (e)

1.8 (re)

<325(e)

357.08 ± 267.2

228.3 ± 160.84

240 ± 100 (e)

Median

0.6 (se)

0.5 (se)

0.9 (se)

#of

Samples

41

54

243

20

15

9

8

10

5

54

239

29

1M

(20 spots)

62

102

40

24 M, 16 F

Analytical

Technique

MS

MS

NAA

PKE

NAA

MS

MS

MS

PDfE

AAS

AAS

85

Reference

Frank etal., 1989

Ngwenya and Turkstra, 1985

Moller and Carlsson, 1984

Curzon and Cutress, 1983

Lappalainen and Knuuttila, 1982

Chaudhari and Crawford, 1981

Cohen etal., 1981

Coles etal., 1980

Lindh and Tveit, 1980

Lappalainen and Knuuttila, 1979

Location

France

South Africa

Sweden

USA

Finland

Australia

England

Finland

Area

Strasbourg

3 Areas

*3 Ethnic groups

New York City

5 Areas

Age

yrs

10-27

32-65

Children

10-76

10-72

Sample

Prep

n

d

d

d

d

d

*

d

Range

152-203 (d)

133 - 180 (e)

102.0- 165.0 (cd)

83.0 - 533.0 (cd)

126-276 (e)

50.0- 999.0 (d)

100-300 (e)

200- 900 (d)

676-702 (e)

133 - 5600

Mean

228.1 ± 152.7 (se)

69.7 ± 19.5 (ie)

147.3 ± 27.3 (peed)

169.3 ± 26.6 (med)

234.5 ± 54.2 (ped)

142.0 ±31.1 (perd)

263.8 ± 67.7 (prd)

261.6 ±188.6 (ie)

115.9 ± 94.4 (ie)

158.2 ± 28.8 (peed)

190.9 ± 38.7 (med)

325.9 ± 107.6 (ped)

153.4 ±24.9 (perd)

359.3 ±161.4 (prd)

135.1 ± 21.2 (cd)

163.0 ± 120.0 (cd)

210 (e)

157.0 ± 87.9 (d)

103

690 (e)

182 ±37.1

Median

141

#of

Samples

8

7

11

12

123

72M.51F

15

37?

1M

(20 spots)

124

Analytical

Technique

XRF

AAS

PKE

AAS

PKE

AAS

PKE

AAS

86

Reference

Cutress, 1979

Curzon and Crocker, 1978

Oehmeetal., 1978

Curzon and Crocker, 1978

Location

14 Countries

Area

USA & New Zealand

Norway Urban

USA & New Zealand

Age

yrs

10-20

Teens

10-20

Sample

Prep

d

d

Range

61 - 5400 (se)

9.9 - 806.0 (e)

76-542

0.0- 0.8 (e)

Mean

893 (se)

153.12 (e)

0.08 (e)

Median

576 (se)

#of

Samples

54

336

10

244

Analytical

Technique

MS

MS

V

MS

87

Shoulder f ClavicleGirdle \scapula

Humerus

FrontalParietalTemporal

-Zygoma ticMaxillaMandible7th cervical vertebra

..-- 1st thoracic vertebra1st nb

Sternum

. .. 12th rib

ForearmIlium |P u b i s 1 Os coxaeIschiumj

Metatarsus•v{\ Phalanges

Figure 1: Bones of the Human Skeleton (Ref. Dorland's Medical Dictionary,W.B. Saunders Co., Philadelphia, PA, 1965).

Dentine

Figure 2: Component tissues of a tooth (Ref. Biochemist's Handbook,Long C. (Ed), Van Norstrand Co, New York, 1961).

CUT

icm

ISOTOPIC RATIOANALYSIS (TIHS)

TOTAL LEAO(IDKS)

TOTAL LEADANA1YSI8(GfAAfl)

Vertical and transverse cuts with stainlesssteel Sagittal Saw (3M Co. Ltd.). Rinsed withultra-pure water; frozen until dissection.

In Class-100Cleanroom: Non-osseousmaterial removed, biopsy cut into 5 or moreslices.

Water-jet, dental probes, compressed gas toremove red/white marrow.

Cortical bone trimmed by osteotome/scalpelblade

Ultra-pure / water wash, then shake withglass-distilled acetone (1 min) and ultra-purewater (1 min), in Teflon vials. Dry withcompressed N2-

Random division of 2 bone types, drived invacuum desiccator in Teflon vials.

Sealed and transported to analyticallaboratory.

Figure 3: Dissection and preparation of cortical and trabecular bone samplefrom a iliac crest bone biopsy {Ref. Inskip et al. Neurotoxicology 13(1992)825}.

NEXT PAGE(S)left BLANK

REFERENCES

AKESSON, K., GRYNPAS, M.D., HANCOCK, R.G.V., ODSELIUS, R, OBRANT, K.J. Energy-dispersivex-ray microanalysis of the bone mineral content in human tabecular bone: a comparison with the ICPES andneutron activation analysis, Calcif. Tissue Int., 55 (1994) 236-239.

AALBERS, TH.G., HOUTMAN J.P.W., MAKKINK, B., Trace-element concentration in human autopsytissue, Clin. Chem., 33 (11) (1987) 2057-2064.

AL-NAIML T., EDMONDS, M.I., FREMLIN, J.H., The distribution of lead in human teeth, using chargedparticle activation analysis, Phys. Med. Biol., 25 (1980) 719-726.

BARANOWSKA, I., CZERNICKI, K., ALEKSANDROWICZ, R, The analysis of lead, cadmium, zinc,copper, and nickel content in human bones from the Upper Silesian industrial district, Sci. Total Environ.,159 (1995) 155-162.

BERCOVITZ, K., HELMAN, J., PELED, M., LAUFER, D., Low lead level in teeth in Israel, Sci. TotalEnviron., 136 (1993) 135-141.

BERCOVITZ, K., LAUFER, D., Carious teeth as indicators to lead exposure, Bull. Environ. Contam. Tox.,50 (1993) 724-729.

BERCOVITZ, K., LAUFER, D., Lead accumulation in teeth of patients suffering from gastrointestinal ulcers,Sci. Total Environ., 101 (1991) 229-234.

BOGDANOVICH, E., KRISHNAN, S.S., LUI, S.M., HANCOCK, R, PEI, Y., HERCZ, G. andHARRISON, J.E., Non-destructive bone aluminum assay by neutron activation analysis, J. Radioanal. Nucl.Chem., 164 (1992) 293-302.

BROADWAY, J.A., STRONG, A.B., Radionuclides in human bone samples, Health Physics, 45 (3) (1983)765-768.

BUSH, V J., MOYER, T.P., BATTS, K.P., PARISI, IE., Essential and toxic element concentrations in freshand formalin-fixed human autopsy tissues, Clin. Chem., 41 (2) (1995) 284-294.

BYRNE, A.R, VRBIC, V., The vanadium content of human dental enamel and its relationship to caries, J.Radioanal. Chem., 54 (1-2) (1979) 77-85.

CHAUDHRI, M.A., AINSWORTH, T., Application of PIXE to studies in dental and mental health, Nucl.Instr. Methods, 181 (1981) 333-336.

CLEYMAET, R, RETIEF, D.H., QUARTER, E., SLOP, D., COOMANS, D., MICHOTTE, Y., Acomparative study of the lead and cadmium content of surface enamel of Belgian and Kenyan children, Sci.Total Environ., 104 (1991) 175-189.

COHEN, D.D., CLAYTON, E., AINSWORTH, T., Preliminary investigations of trace element concentrationin human teeth, Nucl. Instr. Methods, 188 (1981) 203-209.

COLES, S., FLETCHER, R.P., STACK, M.V., Lead, zinc, cadmium and copper in mature and immatureteeth, J. Dent. Res., 59 (1980) 1845.

93

CUA, F.T., HALL, G.S., Trace-element analysis of human teeth and bone by proton-induced x-ray emission,Biol. Trace Elem. Res., 12 (1987) 133-142.

CURZON, M.E.J., CROCKER, D.C., Relationships of trace elements in human tooth enamel to dental caries.Arch. oral. Biol., 23 (1978) 647-653.

CURZON, M.E.J., LOSSE, F.L., Dental caries and trace element composition of whole human enamel:western United States, J. Amer. Dent. Assoc, 96 (1978) 819-822.

CUTRESS, T.W., A preliminary study of the microelement composition of the outer layer of dental enamel,Caries Res., 13 (1990) 73-79.

DEIBEL, M.A., SAVAGE, J.M., ROBERTSON, J.D., EHMANN, W.D., MARKESBERRY, W.R, Leaddeterminations in human bone by particle induced x-ray emission and graphite furnace atomic absorptionspectrometry, I Radioanal. Nucl. Chem., 195 (1) (1995) 83-89.

EDWARD, J., Ion exchange behavior of fresh human bone, J. Radioanal. Nucl. Chem., 144 (1990) 317-322.

EDWARD, J.B., BENFER, RA., MORRIS, J.S., The effects of dry ashing on the composition of human andanimal bone, Biol. Trace Elem. Res., 25 (1990) 219-231.

EICHHORN, K., KNOBUS, B., ROSENKRANZ, G., TELKAMP, H., Radiol Diagn, 21 (1980) 714-720.

EMSLANDER, N., Ludwig-Max Univ Miinchen, Dissertation, (1978).

ERKKILA, J., RIIHIMAKI, V., STARCK, J., PAAKKARI, A., KOCK, B., In vivo measurements of leadin bone (Proc. Int. Symp. In Vivo Body Composition Studies, Toronto, June 1989), In: Advances in In VivoBody Composition Studies, YASUMURA, S., HARRISION, J.E., MCNEILL K.G., WOODHEAD, A.D.AND DILMANIAN, F.A. (Eds), Plenum Press, New York, (1990) 263-265.

FERGUSSON, J.E., PURCHASING, The analysis and levels of lead in human teeth: A Review, Environ.Pollut.,46 (1987) 11-44.

FISENNE, I.M., PERRY, P.M., WELFORD, G.A., Determination of uranium isotopes in human bone ash,Anal. Chem., 52 (1980) 777-779.

FISENNE, I.M., PERRY, P.M., CHU, N.Y., HARLEY, N.H., Measured 234,238U and fallout 239,240Puin human bone ash from Nepal and Australia: skeletal alpha dose, Health Physics, 44 (1) (1983) 457-467.

FISENNE, I.M., LELLER, H.W., PERRY, P.M., Uranium and 226Ra in human bones from Russia, HealthPhysics, 46 (1984) 438-440.

FRANK, R.M., SARGENTINI-MAIER, M.L., TURLOT, J.C., LEROY, M.J.F., Zinc and strontiumanalyses by energy dispersive x-ray fluorescence in human permanent teeth, Archs. Oral Biol., 34 (8) (1989)593-597.

FRANK, R.M., Comparison of lead level in human permanent teeth from Strasbourg, Mexico City and ruralzones of Alsace, J. Dent. Res., 69 (1990) 90-93.

GARANT, P.R., Immuno-electron microscopic study of antigenic surface components of actinomycesnaeslundii in human dental plaque, Archs. Oral Biol., 24 (1979) 369-377.

94

GAWLIK, D., The suitability of iliac crest biopsy in the element analysis of bone and marrow, J. Clin. Chem.Clin. Biochem., 20 (1982) 499-507.

GAWLIK, D., BEHNE, D., BRAETTER, P., GATSCHKE, W. GESSNER, H., J. Clin. Chem. Clin.Biochem., 18 (1982) 403-406.

GIL, F., PEREZ, M.L., FACIO, A., VILLANUEVA, E., TOJO, R., GIL, A., Dental lead levels in theGalician population, Spain, Sci. Total Environ., 156 (1994) 145-150.

GRANDJEAN, P., JORGENSEN, P J., Retention of lead and cadmium in prehistoric and modern humanteeth, Environ. Res., 53 (1990) 6-15.

GRANDJEAN, P., NIELSEN, O.V., SHAPIRO, I.M., Lead retention in ancient Nubian and contemporarybones, J. Environ. Pathol. Toxicol., 2 (1979) 781-787.

GROBLER, S.R., Lead levels in circumpulpal dentine of children from different geographic areas, Archs.OralBiol., 30 (1985) 819-820.

GRYNPAS, M.D., PRITZKER, K.P.H., HANCOCK, R.G.V., Neutron activation analysis of bulk andselected trace elements in bones using a low flux slowpoke reactor, Biol. Trace Elem. Res., 13 (1987) 333-344.

HENSHAW, D.L., HATZIALEKOU, U., RANDLE, P.H., WILLS, H.H., Analysis of alpha particleautoradiographs of bone samples from adults and children in the UK at natural levels of exposure, Radiat.Prot. Dos., 22 (4) (1988) 231-242.

HISANAGA, A., HIRATA, M., TANAKA, A., ISHINISHI, N., EGUCHI, Y., Variation of trace metals inancient and contemporary Japanese bones, Biol. Trace Elem. Res., 22 (1989) 221-231.

HU, H., Distribution of lead in human bone: I. atomic absorption measurements (Proc. Int. Symp. In VivoBody Composition Studies, Toronto, June 1989), In: Advances in In Vivo Body Composition Studies,Yasumura, S., Harrision, J.E., McNeill K.G., Woodhead, A.D. and Dilmanian, F.A. (Eds), Plenum Press, NewYork, (1990)267-274.

HUTIN, M.F.,NETTER, P., BURNEL, D.,GAUCHER, A., Rhumatologie, 12 (1982) 199-203.

HYVONEN-Dabek, M., RAISANEN, J., DABEK, J.T., Proton-induced prompt gamma-ray emission fordetermination of light elements in human bone, J. Radioanal. Chem., 63 (1981) 367-378.

HYVONEN-DABEK, M., Trace element study of human bone by x-ray emission analysis using an externalproton beam, J. Radioanal. Chem., 63 (1) (1981) 163-175.

HYVONEN-DABEK, M., RIHONEN, M., DABEK., Elemental analysis of bone mineral by back scatteringof alpha particles, Phys. Med. Biol., 24 (5) (1979) 988-998.

IGARASHI, Y., YAMAKAWA, A., IKEDA, N., Distribution of uranium in human bones, Radioisotopes,36 (1987) 563-567.

International Commission on Radiological Protection (ICRP), Part 1. Limits for Intakes of Radionuclides byworkers, Pergamon Press, Oxford, 30 (1) (1979) .

95

JAKSIC, M., FAZINIC, S., KRMPOTIC-NEMANIC, I , BUDNAR, M., SMIT, S.,VALKOVIC, V.,Distribution of trace metals in human nasal cavity bones, Nucl. Instr. Methods Phys. Res., B22 (1987) 193-195.

JASIM, F., Some observations on the use of a new matrix modification electrothermal atomization-atomicabsorption spectrophotometric method for the determination of micro and sub-microgram amounts ofmolybdenum in human teeth, Microchem. J., 38 (1988) 337-342.

JAWOROWSKI, Z., BARBALAT, F., BLAEST, C , PEYRE, E., Heavy metals in human and animal bonesfrom ancient and contemporary France, Sci. Total Environ., 43 (1985) 103-126.

JOHANSSON, E., Selenium and its protection against the effects of mercury and silver, J. Trace Elem.Electrolytes Health Dis., 5 (1991) 273-274.

KANEKO, Y., INAMORI, I., NISHIMURA, M., Zinc, lead, copper and cadmium in human teeth fromdifferent geographical areas of Japan, Bull. Tokyo Dent. Coll., 15 (1974) 233-243.

KATIC, V., VUJICIC, G., IVANKOVIC, D., STAVLJENIC, A., VUKICEVIC, S., Distribution of structuraland trace elements in human temporal bone, Biol. Trace Elem. Res., 29 (1991) 35-43.

KEINONEN, M., The isotopic composition of lead in man and the environment in Finland 1966-1987:isotope ratios of lead as indicators of pollutant source, Sci. Total Environ., 113 (1992) 251-268.

KHADEKAR, R.N., RAGHUNATH, R, MSHRA, U.C., Lead levels in teeth of an urban Indian population,Sci. Total Environ., 58 (1986) 231-236.

KHANDEKAR, R.N., ASHAWA, S. C, KELKAR, D.N., Dental lead levels in Bombay inhabitants, Sci.Total Environ., 10 (1978) 129-133.

KNIEWALD, G., KOZAR, S., BRAJKOVIC, D., BAGI, C, BRANICA, M., Trace metal levels in fossilhuman bone from the Bezdanjaca necropolis in Croatia, Sci. Total Environ., 151 (1994) 71-76.

KNUUTTILA, M., LAPPALAINEN, R.A., OLKKONEN, H.5 LAMMI, S., ALHAVA, E.M., Cadmiumcontent of human cancellous bone, Arch. Environ. Health, 37 (5) (1982) 290-294.

KNUUTTILA, M., LAPPALAINEN, R., LAMMI, S., ALHAVA, E., OLKKONEN, H., Chem.-Biol.Interactions, 40 (1982) 77-83.

KNUUTTILA, M., LAPPALAINEN, R, ALAKUJJALA, P., Relationships between carbonate, sex and othermacroelements inhuman whole enamel, Scand. J Dent. Res., 93 (1993) 1-3.

KOLLMEIER, H., SEEMANN, J., WITTIG, P., THIELE, H., SCHACH, S., Altersabhangige Kumulationvon Blei in den Zahnen, Klin. Wochenschrift, 62 (1984) 826-831.

KOSUGI, H., HANIHARA, K, SUZUKI, T., HONGO, T., YOSHINAGA, J., MORITA, M., Elevated leadconcentrations in Japanese ribs of the Edo era (300-120 BP), Sci. Total Environ., 76 (1988) 109-115.

KOWAL, W.A., KRAHR, BEATTIE, O.B., Lead levels in human tissues from the Franklin forensic project,Int. J. Environ. Anal. Chem., 35 (1989) 119-26.

96

LANGMYHR, F.J., SUNDLI, A., JONSEN, J., Atomic absorption spectrometric determination of cadmiumand lead in dental material by atomization directly from the solid state, Anal. Chim. Acta, 73 (1974) 81-85.

LAPPALAINEN, R, KNUUTTILA, M., The distribution and accumulation of Cd, Zn, Pb, Cu, Co, Ni, Mn,and K in human teeth from five different geological areas of Finland, Archs. Oral Biol., 24 (1979) 363-364.

LAPPALAINEN, R, KNUUTTILA, M., Atomic absorption spectrometric evidence of relationship betweensome cationic elements in human dentine, Archs. Oral Biol., 27 (1982) 827-830.

LAPPALAINEN, R, KNUUTTILA, M., LAMM, S., ALHAVA, E.M., Acta Orthop. Scand., 53 (1982)51-55.

LIANQING, L., GUIYUN, L., Uranium concentration in bone of Beijing (China) residents, Sci. TotalEnviron., 90 (1990) 267-272.

LIESE, TH., Dissertation, Univ. of Berlin, (1982).

LIN, L-Q, Trace elements in human bone in the Beijing area by neutron activation analysis, Chung-Hua YuFang i Hsueh Tsa Chih, 22 (2) (1988) 98-100.

LINDH, U., TVEIT, B., Proton microprobe determination of fluorine depth distributions and surfacemultielement characterization in dental enamel, J. Radioanal. Chem., 59 (1) (1980) 167-191.

LINDH, U., The nuclear microprobe applied to bioenvironmental studies, Nucl. Instr. Methods, 181 (1981)171-178.

MOLLER, B., CARLSSON L.E., Particle-induced x-ray emission (PDCE) analysis of trace elements in humancoronal dentin, Swed. Dent. J., 8 (1984) 67-72.

MAENHAUT, W., Bull. Soc. Chim. Belg., 90 (1981) 115-125.

MAHANTI, H.S., BARNES, M., Determination of major, minor and trace elements in bone by inductively-coupled plasma emission spectrometry, Anal. Chim. Acta, 151 (1983) 409-417.

MALIK, S., FREMLIN, J.H., A study of lead distribution in human teeth using charged particle activationanalysis, Caries Res., 8 (1974) 283-292.

MANEA-KRICHTEN, M., PATTERSON, C, MILLER, G., SETTLE, D., EREL, Y., Comparative increasesof lead and barium with age in human tooth enamel, rib and ulna, Sci. Total Environ., 107 (1991) 179-203.

NARAYAN, P.S., DAVID B.B., MCDONALD E.W., Macro-distribution of naturally occurring a-emittingisotopes of U in the human skeleton, Health Physics, 52 (1987) 769-773.

NGWENYA, M. P., TURKSTRA, J., A comparative study of essential biological trace elements in humantooth enamel and dentine obtained from different ethnic groups in south Africa, J. Trace Microprobe Tech.,3 (1-2) (1985) 67-76.

NICHOLSON, J.R.P., SAVORY, M.G., SAVORY, I , WILLS, M.R, Micro-quantity tissue digestion formetal measurements by use of a microwave acid-digestion bomb, Clin. Chem., 35 (3) (1989) 488-490.

97

NIEBERGALL, K., BRAUER, H., GORNER, W., VOGEL, A., KRAMER, R, ZWANZIGER, H., ThirdInt. Meet. Nuclear Anal. Methods, Dresden (1983).

NIESE, S., GORNER, W., VOGEL, A., KRAMER, R, ZWANZIGER, H., Unpublished results, (1982).

NOWAK, B., Occurrence of heavy metals and sodium, potassium,'and calcium in human teeth, Analyst, 120(1995) 747-750.

O'CONNOR, B.H., KERRIGAN, G.C., TAYLOR, K.R, MORRIS, P.D., WRIGHT, C.R, Levels oftemporal trends of trace element concentrations in vertebral bone, Arch. Environ. Health, 35 (1980) 21-28.

OEHME, M., LUND, W., JONSEN, X, The determination of copper, lead, cadmium and zinc in human teethby anodic stripping voltammetry, Anal. Chim. Acta, 100 (1978) 389-398.

OGAWA, K, A study of trace elements in human dental tissues. On concentrations of copper and lead, ShikaIzaku, 46 (1983) 66-78.

PANDAY, V.K., Certain trace elements in normal human bone, Bull. Radiat. Prot., 4 (1981) 11-15.

PIERTA, R., FORTANER, S., SABBIONI, E., GALLORINI, M., Use of Chelex 100 resin inpreconcentration and radiochemical separation neutron activation analysis applied to environmentaltoxicology and biomedical research, J. Trace Micr. Res., 11 (1-3) (1993) 235-250.

PINCHIN, M.J., NEWHAM, J., THOMPSON, R.J.P., Lead, copper and cadmium in normal and mentallyretarded children, Clin. Chim. Acta, 85 (1978) 89-94.

PURCHASE, N.G., FERGUSSON, J.E., Lead in teeth: the influence of teeth type and the sample within atooth on lead levels, Sci. Total Environ., 52 (1986) 239-250.

ROBERTSON, J.D., SAMUDRALWAR D.L., MARKESBERY, W.R, Ion beam analysis of the bone tissueof Alzheimer's disease patients, Nucl. Instr. Methods Phys. Res., B64 (1992) 553-557.

SAMUDRALWAR, D.L., ROBERTSON, J.D., Determination of major and trace elements in bones bysimultaneous PIXE/PIGE analysis, J. Radioanal. Nucl. Chem., 169 (1) (1993) 259-267.

SAMUELS, E.R, MERANGER, J.C., TRACY, B.L., SUBRAMANIAN, K.S., Lead concentrations inhuman bones from the Canadian population, Sci; Total Environ., 89 (1989) 261-269.

SHAPIRO, I.M., MITCHELL, G, DAVIDSON, I., KATZ, S.H., The lead content of teeth: Evidenceestablishing new minimal levels of exposure in a living preindustrial human population, Arch. Environ.Health, 30 (1975) 483-486.

SMYTHE, W.R., ALFREY, A.C., CRASWELL, P.W., CROUCH, C.A., IBELS, L.S., KUBO, H.,NUNNELLEY, L.L., RUDOLPH, H., Trace element abnormalities in chronic uremia, Annals hit. Med., 96(1982)302-310.

SOMERVAILLE, L.J., CHETTLE, D.R., SCOTT, M.C., TENNANT, D.R., MCKIERNAN, M.J.,SKILBECK., A., TRETHOWAN, W.N., hi vivo tibia lead measurements as an index of cumulative exposurein occupationally exposed subjects, Br. J. Ind. Med., 45 (1988) 174-181.

98

SOMERVAILLE, L.J., CHETTLE, D.R., SCOTT, M.C., AUFDERHEIDE, A.C., WALLGREN, IE.,WITMERS, L.E., RAPP, G.R, Comparison of two in vitro methods of bone lead analysis and the implicationfor in vivo measurements, Phys. Med. Biol., 31 (11) (1986) 1267-1274.

STACK, M.V., BURKITT, A.J. NICKLESS, G., Characterization of teeth by trace elements, Int. J. ForensicDent., 5 (1974) 62-65.

STACK, M.V., Lead, zinc and cadmium concentrations in Romano-British teeth, J. Dent. Res., 61 (4) (1982)563.

STEENHOUT, A., POURTOIS, M., Lead accumulation in teeth as a function of age with differentexposures, Br. J. Ind. Med., 38 (1981) 297-303.

STEIN, G., ANKE, M., FUNFSTUCK, R, SCHNEIDER, H.J., Z. ges. inn. Med., 34 (1979) 648-651.

STREHLOW, CD., KNEIP, T.J., The distribution of lead and zinc in the human skeleton, Amer. Ind.Hygiene Assoc, 30 (1969) 372-378.

SUZUKI, Y., TOHOKU J. Exp. Med., 129 (1979) 327-336.

TAKIZAWA, Y., ZHAO, L., YAMAMOTO, M., ABE, T., UENO, K., Determination of 210Pb and 210Poinhuman tissue of Japanese, J. Radioanal. Nucl. Chem., 138 (1) (1990) 145-152.

United Nations Scientific Committee on the Effects of Atomic Radiation (UNSCEAR), Sources and effectsof ionizing radiation, United Nations, New York (1982).

VALKOVIC, V., JAKSIC, M., KRMPOTIC-NEMANIC, J., Distribution of trace elements within bonesin nasal cavity and labyrinth in human, Biol. Trace Elem. Res., 12 (1987) 375-381.

VRBIC, V., STUPAR, J., BYRNE, A.R., Trace element content in primary and permanent tooth enamel,Caries Res., 21 (1987) 37-39.

WARD, N.I., The determination of boron in biological materials by neutron irradiation and prompt gamma-ray spectrometry, J. Radioanal. Nucl. Chem., 110 (2) (1987) 633-639.

WIELOPOLSKI, L., ROSEN, J.F., SLATKIN, D.N., VARTSKY, D., ELLIS, K.J., COHN, S.H., Med.Phys., 10(1983)248-251.

WILKINSON, D.R., PALMER, W., Lead in teeth as a function of age, Am. Lab., 7 0 67-70.

WITTMERS, L.E., ALICH, A., AUFDERHEIDE, A.C., Am. J. Clin. Pathol., 75 (1981) 80-85.

WRENN, M.E., DURBIN, P.W., HOWARD, B., LIPSZTEJN, X, RUNDO, J., STELL, E.T., WILLIS, D.L,Metabolism of ingested U and Ra5 Health Physics, 48 (1985) 601-633.

YAMADA, M-O., Accumulation of mercury in excavated bones of two natives in Japan, Sci. Total Environ.,162 (1995) 253-256.

YOSHINAGA, J., SUZUKI, T., MORITA, M., HAYAKAWA, M., Trace elements in ribs of elderly peopleand elemental variation in the presence of chronic diseases, Sci. Total Environ., 162 (1995) 239-252.

99

YOSHINAGA, J., SUZUKI, T., Sex- and age-related variation in elemental concentrations of contemporaryJapanese ribs, Sci. Total Environ., 79 (1989) 209-221.

ZAICHICK, V.Y., Instrumental activation and x-ray fluorescent analysis of human bone in health anddisease, J. Radioanal. Nucl. Chem., 179 (2) (1994) 295-303.

ZWANZIGER, H., The multielement analysis of bone: A review, Biol. Trace Elem. Res., 19 (1989) 195-231.

ZWANZIGER, H., GORNER, W., VOGEL, A., KRAMER, R., Submitted for publication in 1987, Calcif.Tissue Int., (1987).

ZWANZIGER, H., VOGEL, A., KRAMER, R., GORNER, W., NIEBERGALL, K., BRAUER, H., ZFK-Report,524 (1985) 317-322.

100