Top Banner
1 ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS L.M. SPASOVA, M.I. OJOVAN Immobilisation Science Laboratory, Department of Materials Science and Engineering, University of Sheffield, United Kingdom Abstract A summary is presented of the potential of non-destructive acoustic emission (AE) method to be applied for structures immobilising nuclear wastes. The use and limitations of the method are discussed with given examples of experimental configurations and results obtained from AE monitoring and data analysis of two different processes addressing particular issues related to the nuclear waste immobilisation. These are (a) corrosion of aluminium, classified as intermediate level waste (ILW) in the UK, encapsulated in cementitious structures and (b) partial melting and solidification during cooling of granite at a pressure of 0.15 GPa which simulates the conditions in a deep borehole disposal of canisters of vitrified high level waste (HLW). Methodology for analysis of the collected data and characterisation of the potential AE sources is performed at different steps including simple signals count and more complex signal parameter-based approach and advanced signal processing. The AE method has been shown as a potential tool for monitoring and inspection of structures immobilising nuclear wastes in relation to the time progress of different interactions of the waste with the encapsulating matrix or the wasteform with the hosting environment for permanent disposal. 1. INTRODUCTION Over a number of years in the UK the encapsulation of low and intermediate level radioactive waste (LILW) in composite cements has been operated in an industrial scale resulting in the manufacturing of tens of thousands of containers with cementitious wasteforms [1]. Composite cement formulations with a partial replacement of ordinary Portland cement (OPC) by blast furnace slag (BFS) or pulverized fuel ash (PFA) have been used to encapsulate liquid and solid ILW such as sludges, ion exchange resins and metallic debris [2, 3]. The produced cementitious wasteforms have been sealed in 500-litre drums [4] and placed in interim storage for minimum of 50 years before final disposal [3]. The mechanical stability of the encapsulating cementitious structures over the long period of interim storage can be substantially affected by chemical and electrochemical interactions of the waste with the host matrix [3]. A particular issue is the corrosion of reactive metals such as aluminium encapsulated in BFS composite cements [5, 6] causing cracking of the structures as a result of the accumulation of corrosion products and hydrogen gas generation and release. According to the latest UK Radioactive Waste Inventory Report [1], there are 980 tonnes of aluminium classified as ILW, accumulated at nuclear sites in the country as legacy waste. Given the scale of that figure the cementation of aluminium and the safe storage of the packaged wasteforms along with the capability to assess their acceptability for transportation and final disposal are important issues for the nuclear industry needed solutions. Alternative cement-based formulations such as calcium sulfoaluminate cements, condensed silica fume and sulphate resisting Portland cements have been studied to reduce the corrosion of aluminium [3, 7]. Non-intrusive methods for continuous monitoring and inspection, described in this paper, would provide unique information for the mechanical performance of the sealed cementitious structures in relation to the initiation and time progress of the aluminium corrosion.
14

ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS Sheffield... · ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS L.M. SPASOVA, M.I. OJOVAN Immobilisation Science Laboratory,

Mar 18, 2020

Download

Documents

dariahiddleston
Welcome message from author
This document is posted to help you gain knowledge. Please leave a comment to let me know what you think about it! Share it to your friends and learn new things together.
Transcript
Page 1: ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS Sheffield... · ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS L.M. SPASOVA, M.I. OJOVAN Immobilisation Science Laboratory,

1

ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS

L.M. SPASOVA, M.I. OJOVAN

Immobilisation Science Laboratory, Department of Materials Science and Engineering, University of Sheffield, United Kingdom

Abstract

A summary is presented of the potential of non-destructive acoustic emission (AE) method to be applied for structures immobilising nuclear wastes. The use and limitations of the method are discussed with given examples of experimental configurations and results obtained from AE monitoring and data analysis of two different processes addressing particular issues related to the nuclear waste immobilisation. These are (a) corrosion of aluminium, classified as intermediate level waste (ILW) in the UK, encapsulated in cementitious structures and (b) partial melting and solidification during cooling of granite at a pressure of 0.15 GPa which simulates the conditions in a deep borehole disposal of canisters of vitrified high level waste (HLW). Methodology for analysis of the collected data and characterisation of the potential AE sources is performed at different steps including simple signals count and more complex signal parameter-based approach and advanced signal processing. The AE method has been shown as a potential tool for monitoring and inspection of structures immobilising nuclear wastes in relation to the time progress of different interactions of the waste with the encapsulating matrix or the wasteform with the hosting environment for permanent disposal.

1. INTRODUCTION

Over a number of years in the UK the encapsulation of low and intermediate level radioactive waste (LILW) in composite cements has been operated in an industrial scale resulting in the manufacturing of tens of thousands of containers with cementitious wasteforms [1]. Composite cement formulations with a partial replacement of ordinary Portland cement (OPC) by blast furnace slag (BFS) or pulverized fuel ash (PFA) have been used to encapsulate liquid and solid ILW such as sludges, ion exchange resins and metallic debris [2, 3]. The produced cementitious wasteforms have been sealed in 500-litre drums [4] and placed in interim storage for minimum of 50 years before final disposal [3].

The mechanical stability of the encapsulating cementitious structures over the long period of interim storage can be substantially affected by chemical and electrochemical interactions of the waste with the host matrix [3]. A particular issue is the corrosion of reactive metals such as aluminium encapsulated in BFS composite cements [5, 6] causing cracking of the structures as a result of the accumulation of corrosion products and hydrogen gas generation and release. According to the latest UK Radioactive Waste Inventory Report [1], there are 980 tonnes of aluminium classified as ILW, accumulated at nuclear sites in the country as legacy waste. Given the scale of that figure the cementation of aluminium and the safe storage of the packaged wasteforms along with the capability to assess their acceptability for transportation and final disposal are important issues for the nuclear industry needed solutions. Alternative cement-based formulations such as calcium sulfoaluminate cements, condensed silica fume and sulphate resisting Portland cements have been studied to reduce the corrosion of aluminium [3, 7]. Non-intrusive methods for continuous monitoring and inspection, described in this paper, would provide unique information for the mechanical performance of the sealed cementitious structures in relation to the initiation and time progress of the aluminium corrosion.

Page 2: ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS Sheffield... · ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS L.M. SPASOVA, M.I. OJOVAN Immobilisation Science Laboratory,

2

Non-destructive and remote operating methods for testing and evaluation could be also beneficial for monitoring and understanding the potential interactions of the waste packages with the surrounding environment. This paper reports an example of acoustic emission (AE) monitoring and characterisation of the processes of partial melting and solidification of granite as envisaged host environment for canisters of vitrified HLW.

According to one of the very deep borehole disposal concepts, developed by Gibb [8], cylindrical canisters of HLW as those produced in the UK [3, 4] will be placed in boreholes drilled in granitic continental crust at a depth of 4-5 km. As a result of the natural decay of the present radionuclides [9] the temperature of the waste packages and consequently around the containers will be high enough to partially melt the surrounding granite. Over time the containers gradually will cool down allowing the granite melt to recrystallise and seal the containers into a sarcophagus of solid granite, preventing sinking of the packages. For the purpose of the proposed disposal scheme the generated and detected AE signals would provide important information for the mechanisms associated with the dynamics of this type of transformations difficult for monitoring and evaluation under the predicted conditions of high pressure and temperature deep underground.

Furthermore similar principle of melting of the surrounding granite due to radiogenic heat followed by solidification/recrystallisation of the melt has been proposed as a potential option for disposal of highly radioactive sealed radioactive sources (SRS) [10] or to investigate the deep interior of the Earth crust [11]. As reported in [10, 11] detected acoustic signals as a result of interactions of the radioactive waste with the surrounding environment would be an effective way to track specially designed self-descending capsules with SRS and transmit to the surface new information for the seismic activity, structure and formation of deep layers in the Earth. However, the theoretical calculations and conclusions drawn in [8 - 11] need to be validated by experimental data.

This paper summarises and discusses the major findings of conducted AE studies on cementitious structures with encapsulated aluminium and partial melting and solidification of natural granite likely to occur in a very deep borehole for disposal of containers of HLW.

2. ACOUSTIC EMISSION METHOD

Acoustic emission is a natural occurring phenomenon associated with release of stress energy in the form of transient waves (typically in the frequency range of 20 kHz to 1.2 MHz [12]) due to irreversible mechanical changes within materials and structures. The largest scale AE sources are the seismic events whereas the smallest processes that still generate detectible AE signals are microscopic defect movements in the order of a few picometres [12] in a stressed structure. Sources of AE are also chemical reactions leading to physical changes, e.g., cement hydration [13], electrochemical processes such as corrosion of metals [14] or fracture initiation and development and plastic deformation of various materials and structures during compression or tensile loading, fatigue or hydraulic tests [12, 15].

Over the last 30 years in parallel with the developments in the sensor technology and microelectronics a non-destructive method based on detection and processing of AE signals has been developed and implemented in a large number of areas from civil engineering to orthopedics [12, 15, 16]. The basic chain (Fig. 1a) representing the AE wave generation and release, detection, measurement and storage consists of three closely connected components [17]. The first one includes the examined structure with its intrinsic wave propagation characteristics such as attenuation, reflection and absorption determined by the initial composition, microstructure and geometry and the type of the AE source(s). A comprehensive overview of the types of AE sources in various materials can be found in [12, 15]. The second component of the AE chain involves the sensors attached to the structure, their type, number and position followed by preamplifiers used for reliable transmission of the signals to the data acquisition system. The last component is the fully integrated computer-based AE system used for filtering, measurement, analog-to-digital conversion and storage of the acquired signals with high speed and accuracy.

Page 3: ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS Sheffield... · ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS L.M. SPASOVA, M.I. OJOVAN Immobilisation Science Laboratory,

3

An AE signal (or hit) generated from the aluminium corrosion in an OPC structure detected by a piezoelectric transducer, measured and stored by a conventional AE computer-based system is illustrated in Fig. 1b. It is characterised by a number of parameters in a time domain with standardised and broadly accepted definitions as given in [17].

a)

b)

FIG. 1. (a) Schematic of AE signals’ generation, detection and processing and (b) recorded waveform of an acoustic signal with its parameters in a time domain [17].

However, the application of the AE method in the field of nuclear waste management is not completely explored and very limited. The first report for the feasibility for detection of acoustic waves during processing of glass and ceramic for immobilisation of nuclear wastes is published by Belov and Aloy [18]. The authors summarised the main advantages of the AE method to be applied as a tool for quality control emphasizing on its high sensitivity, relatively simple implementation by attachment of stationary detectors with a high radiation and heat resistance and ability to be applied for different materials with varying composition and microstructure [18]. This list of advantages can be extended mentioning that AE is a passive method, i.e., no additional stimuli applied to the examined structure are needed to generate acoustic waves, the monitoring is performed remotely and, in theory, for unlimited interval of time allowing scanning of the overall volume of the structure and providing information for the dynamics and the time progress of the AE activity in real time [17]. Nevertheless the successful application of the AE method requires well defined aims, knowledge and assessment of the type of active AE source(s), the composition and geometry of the examined structure, the experimental conditions associated mainly with the level of the background noise and complementary noise sources, e.g., friction at the contact interface between the testing machine for mechanical loading and the specimen [19], the frequency operational range of the sensors used and the quality of their attachment to the structure. Under conditions of a high temperature, aggressive solution or

Page 4: ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS Sheffield... · ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS L.M. SPASOVA, M.I. OJOVAN Immobilisation Science Laboratory,

4

radioactivity, specially designed sensors or waveguides are needed [12]. All of those factors (determined by the experimental setup) lead to collection of AE signals with diversified parameters and development of relatively complex methods for AE sources location, orientation and energy characterisation such as moment tensor and wavelet [15, 20]. However, the AE technique has achieved a high level of ability and industrial approval in various applications with a large database of experimental setups for a wide range of materials, components and structures and procedures for data analysis [12, 15]. This motivated the ground research work undertaken at the Immobilisation Science Laboratory (ISL) at the University of Sheffield, UK on the feasibility of the AE method to be applied for structures immobilising nuclear wastes focused on corrosion of aluminium encapsulated in cementitious structures [17, 21-23] and partial melting and solidification during cooling of granite samples at a high pressure for the purpose of very deep borehole disposal of vitrified HLW [24].

3. SOURCES OF AE SIGNALS STUDIED IN STRUCTURES APPLIED FOR IMMOBILISATION OF NUCLEAR WASTES

The main types of AE sources detected and characterised to the purpose of nuclear waste immobilisation can be divided in two main groups. The first one are damage initiation and development within cementitious structures (BFS/OPC to mass ratio 7:3 [17] and pure OPC used as a reference [21-23]) due to the corrosion of encapsulated aluminium. The second group of processes responsible for the generation and detection of AE signals are associated with phase transformations as a result of partial melting and solidification during cooling of granite at a temperature of 780 °C and a pressure of 0.15 GPa [24] and defects (microcracks) formation during high temperature processing of glass and ceramic [18].

4. EXPERIMENTAL SETUPS FOR AE MONITORING OF STRUCTURES IMMOBILISING NUCLEAR WASTES

In order to monitor the potential AE sources in nuclear wasteforms the basic characteristics (in terms of AE) of the examined structures and principles established for acoustic wave acquisition, critically examined in [12, 15], have been applied.

For the experiments with cementitious structures encapsulating aluminium laboratory scale units were prepared as described in [17, 21-23]. Considering the high level of attenuation and ultrasonic wave dispersion in concrete, mortar and cement paste [25], and conducted detailed experimental and simulation work on AE from cracking of concrete due to the corrosion of reinforcement [26], a broadband piezoelectric transducer (or sensor) type WD, calibrated and supplied by Physical Acoustics Corporation (PAC), was chosen. The small scale cementitious samples, simulating actual wasteforms, poured and solidified in 340 mL plastic containers (Fig. 2a) after curing in an environmental chamber for 180 days were immersed in deionized water. This condition simulated accelerated corrosion possible to occur due to the penetration of water within the waste packages over the period of interim storage. Before the commencement of the AE monitoring the WD transducer was attached to the bottom of the plastic container (Fig. 2a) and connected with a preamplifier type 2/4/6 from PAC set at 40 dB. Each of the generated by the sensor electrical signals (Fig. 1b) was passed through a bandpass filter, operating between 20 kHz and 3 MHz, set at the PCI-2 AE data acquisition board (Fig. 1a) also calibrated and supplied by PAC. Hit driven data acquisition was established as only signals with an amplitude above 40 dB (or 10 mV) were digitized with a sampling rate of 5 MSPS (mega samples per second) and stored on the hard drive of a conventional PC (Fig. 2a). The set of a threshold level is a standard way to limit the volume of the data collected (or to rectify the noise) [12]. The value of 40 dB applied in this study was chosen based on pre-test monitoring of the background noise characteristics.

Very similar configuration layout of the PCI-2 based AE system (details are given in [17, 21, 24]) was used for processing and recording of electrical signals generated by the WD transducer during partial melting and solidification of a granite sample at a temperature of 780 ºC and a pressure of 0.15 GPa. The initial material with a weight of only 0.86915 g was sealed in a gold capsule and placed at the top

Page 5: ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS Sheffield... · ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS L.M. SPASOVA, M.I. OJOVAN Immobilisation Science Laboratory,

5

end of a vertically mounted cold-seal pressure vessel as shown in Fig. 2b. For this experiment it was required to prevent the sensor from overheating. To that purpose the sensing element was firmly attached, using a G-clamp, to the cold end of the pressure vessel (Fig. 2c) used as a waveguide. This is a common approach for AE monitoring of high temperature processes [12] also used for the experiments of melting and cooling of glass and ceramic samples performed by Belov and Aloy [18].

FIG. 2. Experimental setup for AE data acquisition applied for (a) cementitious samples with encapsulated aluminium [17] and (b) and (c) granite sample sealed in a gold capsule [24].

Unfortunately the lack of information for experimental details for AE detection and data acquisition might hamper the attempts to relate the data obtained in different studies or to repeat the experiments resolving outstanding issues related to the impact of the detector unit and the configuration layout for data collection and processing on the final results. Therefore for consistent AE studies the details of the experimental setup and the approaches applied for data acquisition are equally important as the methodology for post-test data analysis. In relation to the aims of the AE study, e.g., detection of AE activity, source location and orientation factors such as composition and sample preparation, type, number and location of the sensors, threshold level and filters applied as well as the experimental conditions, e.g., steps and level of loading during mechanical tests, presence and type of aggressive solution during corrosion monitoring or temperature and pressure during material processing have to be considered and in many cases their impact assessed via additional data validating experiments. This will allow to conclude on general trends and alterations in the acquired AE signatures.

WD Transducer

Pressure

c)

Furnace

Pressure

b)

a)

Page 6: ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS Sheffield... · ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS L.M. SPASOVA, M.I. OJOVAN Immobilisation Science Laboratory,

6

5. APPROACHES FOR ANALYSIS OF THE AE DATA COLLECTED FROM STRUCTURES APPLIED FOR IMMOBILISATION OF NUCLEAR WASTES

In the field of AE three main approaches for data analysis have been developed and established over the years [27]. The first approach to conclude on the presence of some kind of mechanical events within the structures generating AE waves is based on the total number and rate of the detected acoustic signals above the threshold level. The second approach utilizes the parameters of the recorded signals in time domain such as amplitude, duration, counts and absolute (ABS) energy (Fig. 1b). The third approach involves methods applied for digital signal processing based on the digitized and stored waveforms of the acquired signals. Each of those approaches has advantages and limitation, summarised in Table I, to be considered in conjunction with the aims of the study undertaken. For large scale structures such as bridges the AE hits rate can be an effective way for structural health monitoring [28] but not enough informative for the purpose of characterisation or location of AE sources when the properties of the material (or structure) are examined.

TABLE 1. ADVANTAGES AND LIMITATIONS OF THE APPROACHES FOR AE DATA ANALYSIS

Approach for AE data analysis

Advantages Limitations

Number of AE signals detected above the level of the background noise

Instant alarm to a sudden deterioration of the structure under monitoring and early indication for plastic deformation

No information for the features of the AE source(s) or its location

Analysis of the time domain parameters of the recorded AE signals

Less time and computer resources demanding approach suitable for monitoring of large structures; Can be easily applied for real time monitoring as a good indicator for the presence and severity (micro or macro scale) of the damage induced (the AE sources)

Provide no information for the location of the AE source(s) and less data for its dimension due to the strong dependence of the acoustic parameters on the material composition, geometry, propagation properties, sensors location and quality of coupling

AE signal processing Less dependent on the experimental setup approach but still dependent on the type of the AE source and the propagation properties of the material; Basic approach for AE source location providing complementary information for characteristic features of the AE generation and release

This approach requires large storage space and computational resources; Typically is proceeded after the end of the active monitoring and data collection; Dependant on the damping and/or modulation of the frequency modes present within the AE signal

5.1. Approaches for AE data analysis and major results obtained for the cementitious structures with encapsulated aluminium

The main aims of the AE monitoring of the cementitious samples with encapsulated aluminium were (a) to detect acoustic signals above the threshold level under the established experimental conditions and assess the overall mechanical performance of the structures in relation to the findings of the visual and microscopy observations and (b) to characterise and distinguish (if possible) the potential AE sources. It is well known that the failure of cementitious structures under loading is characterised by detection of a large number (thousands) of AE signals due to microcracks formation and growth and their localisation in a fracture process zone leading to nucleation of visible cracks when the ultimate strength (or peak loading) of the structure is achieved [12, 15, 17, 21, 26].

Page 7: ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS Sheffield... · ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS L.M. SPASOVA, M.I. OJOVAN Immobilisation Science Laboratory,

7

During the experiments conducted for different periods of time (183.5 hours for the BFS/OPC [17] and 51.5 hours for the reference OPC [21, 22] sample with encapsulated aluminium) the first indication for the presence of AE sources and their time depended activity was provided by simply plotting the cumulative number of the recorded AE hits and associated ABS energy.

From the graphs in Figs 3a and 3b it can be seen that in the history of the conducted monitoring of the OPC and BFS/OPC samples with encapsulated aluminium there were periods of very low or almost no AE followed by intervals of time with a high hits rate. Without a need for post-test data analysis it was possible during the active monitoring to resemble a typical response of cementitious structures, showing Kaiser effect [12, 29], and conclude on the presence of macro scale (visible) damage of the samples later confirmed by visual observation. The next step in the methodology for AE data analysis, addressing the second main aim of the study, was to use the time domain parameters of the detected signals directly associated to the strength (in close relation to micro or macro scale of the AE sources) and the relative position of the source(s) toward the sensor. As it can be seen in Figs 3a and 3b according to their amplitude and duration the signals detected respectively for the OPC and BFS/OPC samples with encapsulated aluminium could be divided in two main groups. The first group is represented by a large number of signals with an amplitude below 45 dB and a duration below 250 μs. The second group comprises of essentially less in number signals with an amplitude above 45 dB and a duration more than 250 μs. Precise analysis involving all hits recorded for the cementitious samples was applied in [17, 21, 22]. The criteria of the procedure developed by Wu et al. [30] was used to classify detected populations of signals based on their amplitude, duration and counts and associate their appearing with potential sources of AE such as microcracks initiation and propagation and hydrogen gas release. More than 90% of the total number of AE signals (2328 detected for the BFS/OPC [17] and 5340 for the OPC [17] sample with encapsulated aluminium) were classified in groups and related to cracking of the encapsulating cementitious structures and emissive hydrogen gas generation, friction and release as a result of the aluminium corrosion development.

The final step in the analysis of the recorded AE data was to apply methods of digital signal processing of the collected and stored signal waveforms. This is a well established and effective practice to extract additional information for the frequency characteristics hidden in the time domain representation of the signals. As reported in [17, 23] the main frequency component (or primary frequency) obtained by means of fast Fourier transformation (FFT) (Figs 3d and 3g) of the largest population of signals was at 34 kHz. However, the frequency spectra of the short (duration less than 100 μs) hits, classified based on their time domain parameters, showed also a high intensity for frequencies above 100 kHz (Fig. 3d). The wavelet transformation (WT) applied to resolve in time the frequency modes present in the signal revealed that these low and high frequency components arrived within the first 100 μs of the duration of the recorded hit (Fig. 3e) considered to characterise the source(s) of AE [31]. This type of signals were related to microcracking of the cementitious structures whereas the other large group of recorded acoustic waves with a duration above 100 μs and a dominant low frequency component at 34 kHz (Fig. 3g) were assign to high energy emitting processes such as hydrogen gas evolution due to the corrosion of aluminium and/or visible cracks formation and extension within the encapsulating matrix [17, 21-23].

Page 8: ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS Sheffield... · ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS L.M. SPASOVA, M.I. OJOVAN Immobilisation Science Laboratory,

8

FIG. 3. 3D representation of the amplitude-duration-time correlation of the recorded AE signals for (a) reference OPC and (b) BFS/OPC sample with encapsulated aluminium and (c) and (f) typical

acoustic waveforms, (d) and (g) their frequency and (e) and (h) frequency-time domain characteristics obtained by FFT and WT respectively of signals detected for the OPC sample with encapsulated

aluminium.

4045

5055

6065

0

10

20

30

40

50

0250

500750

10001250

1500

Duratio

n, us

Tim

e, h

rs

Amplitude, dB

4045

5055

6065

020

40

60

80

100

120

140

160

180

200

0250

500750

10001250

1500

Duration, u

s

Tim

e, h

rs

Amplitude, dB

a) b)

Page 9: ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS Sheffield... · ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS L.M. SPASOVA, M.I. OJOVAN Immobilisation Science Laboratory,

9

5.2. Approaches for AE data analysis and major results obtained for partial melting and solidification of a granite sample at a high pressure

During the AE monitoring of the partial melting and solidification of powder of natural granite (E93/7 used for the experiments in [32, 33]) at a pressure of 0.15 GPa the cumulative number of AE hits and their ABS energy (Fig. 4a) did not provide sufficient information to initially distinguish acoustic signals due to potential alteration of the volume and shape of the material and the noise produced by the equipment (Fig. 4b). To that purpose extended AE data analysis based on the time domain parameters of the collected signals for two experiments, conducted with and without a granite sample, was performed [24]. Typically the noise is distinguished by characteristic features [12]. In this study the duration was determined as a distinguishing parameter of the detected AE signals for the granite sample and the noise. Consequently only hits with a duration between 500 µs and 8000 μs detected in large populations during the constant temperature melting of the granite sample at 780 ºC±0.5 ºC (period 2 in Fig. 4a) and solidification (period 3 in Fig. 4a) were used to characterise the monitored transformations within the material. As reported in [24] the transformation of the solid phases in the granite during the constant temperature melting were distinguished by continuous type of AE signals, as shown in Fig. 4c, characterised by a primary frequency mainly at 170 kHz and 268 kHz. The WT analysis (Fig. 4e) of the signal waveform revealed that this hit convey information for closely spaced (in time) events distinguished by a broad range of frequencies (from 20 kHz to 300 kHz) rather than individual bursts of stored mechanical energy. During the relatively fast cooling of the sample, used to allow glass formation from the granite melt (Fig. 4f), AE signals with diversified frequency characteristics (the largest population of signals were characterised by a primary frequency distributed between 200 to 300 kHz [24]) were recorded. Bubbles formation and “cracked interfaces” [33] between the crystals and the glass formed (Fig. 4g) due to their thermal expansion mismatch were suggested as potential sources of AE signals.

Although promising these preliminary results need to be verified by additional experiments and extended for the purpose of a real application with investigation of the major impact of the cooling rate (related to the recrystallisation of the partially melted granite [8-11]) on the characteristics of the recorded AE waves. This is associated with significant increase of the duration of the cooling stage - from less than 24 hours to solidify the partially melted material [24] to more than 300 hours to allow its recrystallisation. AE monitoring is currently under way at the ISL on the recrystallisation of the granite and collecting data for the acoustic noise produced by the equipment.

Note that Belov and Aloy [18] reported only results showing the possibility to detect AE pulses during high temperature processing of different glass and ceramic samples in comparison with the background noise level.

Page 10: ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS Sheffield... · ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS L.M. SPASOVA, M.I. OJOVAN Immobilisation Science Laboratory,

10

FIG. 4. Cumulative number of AE hits and ABS energy recorded during the experiments (a) with a granite sample and (b) without a sample in the pressure vessel, (c) typical acoustic waveform and (d)

its frequency and (e) frequency-time domain characteristics obtained by FFT and WT respectively during the constant temperature melting of the granite solidified into a structure of crystals embedded in a glass matrix observed by (f) plain polarised light and (g) Scanning Electron Microscopy (SEM)

micrograph of the formed bubbles and a potential “cracked interface” between a crystal and the glassy phase.

0 50 100 150 200 250 300 350 400

0

2000

4000

6000

8000

Time, hrs

Cum

ula

tive

Num

ber

of

AE

Hits

0

10000000

20000000

30000000

40000000

50000000

60000000

Cum

ulative A

BS

En

ergy, aJ

0 10 20 30 40 50 60 70 80

0

2000

4000

6000

8000

Time, hrs

Cu

mu

lativ

e N

um

be

r of

AE

Hit

s

0.00E+000

5.00E+007

1.00E+008

1.50E+008

2.00E+008

2.50E+008

3.00E+008

3.50E+008

Cum

ula

tive A

BS

En

ergy, a

J

a) b)

Bubble

Crystal

Glass

f) g)

1 2 3 1 2 3

Page 11: ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS Sheffield... · ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS L.M. SPASOVA, M.I. OJOVAN Immobilisation Science Laboratory,

11

6. DISCUSSION

The studies in [17, 21-24], briefly reviewed in this paper, contributed with new information for a feasible solution for long-term monitoring and assessment of the mechanical performance of packaged radioactive wasteforms without a need for a direct contact, and the time progress and impact of potential interactions of the nuclear waste packages with the surrounding granitic environment for permanent disposal. However, these initial studies have to be further extended as the main logically derived directions are as follows:

AE monitoring and data analysis of the corrosion process of other metals [5, 6] classified as ILW in the UK such as Magnox (magnesium-aluminium alloy) encapsulated in cements;

AE trials on larger (or real scale) inactive wasteforms with encapsulated aluminium or Magnox and monitoring of the background noise needed for additional assessment of the feasibility of the method, the number of sensors needed to monitor the overall structure, the impact of the drum shape and material on the wave propagation and the application of the data collected for AE source location and dimension assessment;

AE trials on active drums with encapsulated metals such as aluminium and Magnox;

Accumulation and comparison of AE data for the partial melting and solidification/recrystallisation of granites, e.g., with different amount of water present, under conditions simulating a very deep borehole for disposal of containers of HLW.

During each of those studies various difficulties may appear that cannot be predicted in advance. However, the AE method has been proven as a valuable tool with a potential to be tailored in a close relation to the aims of the study and the conditions of the surrounding environment.

An obvious concern when applying a passive “listening” of AE signals, used as a main argument against the broad industrial application of the method, is that noise signals may be detected or the information collected is corrupted by sources out of interest. Easy for implementation approaches such as attachment of broadband AE sensors [17, 21-24] and signal filtering or post-test signal parameters analysis can be used to identify features of the background noise and to filter it out. In practice such an approach requires good interpretative skills and may vary from case to case. Another approach to eliminate the effect of “unwanted” signals is to use guard sensors [28] positioned to collect data for the noise (to be subtracted later) rather than AE originating from the monitored region of interest.

Focused attention is also needed to understand the continuous type and the potential sources of AE during melting and glass formation in granites and generally in materials. These fundamental issues with a long history of a discussion require new approaches and AE could be one of them.

However, very important for the successful application of the AE method is to establish and assess the close connection between the three main components of the AE chain as given in Fig. 1a. This is a task involving knowledge from relevant studies, experiments for optimal positioning of the sensors and configuration of the data acquisition layout and, in many cases, the application of complementary diagnostic methods such as ultrasonic damping measurements or microscopy. The results of these techniques will assist in understanding and development of efficient test approaches for industrial applications. Extended work is also needed to analyse and interpret the data collected in order to establish a good correlation between the behavior of the structures over time and their AE response. The cumulative number of AE signals and associated ABS energy could be an effective way to confirm the presence of damage as shown by the study on cementitious structures with encapsulated aluminium [17, 21-23]. For more detailed AE sources characterisation or data filtering the parameters of the signals in time domain or obtained by conventional methods of digital signal processing can contribute for the accurate interpretation of the data collected [17, 21-24].

Page 12: ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS Sheffield... · ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS L.M. SPASOVA, M.I. OJOVAN Immobilisation Science Laboratory,

12

7. CONCLUSIONS

Acoustic emission method offers a number of advantages when applied in the field of nuclear waste management. These are:

High sensitivity;

Potential for continuous and remote monitoring (with waveguides);

Providing information for acoustic waves generation processes;

Potential for AE source location;

No need for additional action on the structures (passive method);

Low costs for long-term implementation.

It also has limitations mainly associated with the presence and level of the background noise and the configuration of experimental setup for AE detection, e.g., number and position of the sensors used.

The reviewed examples of preliminary AE studies addressing important issues in the field of nuclear waste management revealed that the AE method is a feasible option providing flexible and informative solution over long periods of time with supporting publications available [17, 18, 21-24, 35-37]. Although, at the present time, there is a very limited research on AE applied to structures immobilising nuclear wastes and extended work for validation of the method for real structures is required, this could be an area for future development and implementation with promising outcomes.

REFERENCES

[1] The 2004 United Kingdom Radioactive Waste Inventory: Main Report. DEFRA/RAS/05.002, Nirex Report N/090, October 2005.

[2] SHARP, J.H., HILL, J., MILESTONE, N.B., MILLER, E.W., Cementitious systems for encapsulation of intermediate level waste, Proc. ICEM’03 Conf., Oxford, Paper ICEM’03-4554 (2003).

[3] STREATFIELD, R., A review and update of the BNFL cement formulation development programme for the immobilisation of intermediate level wastes from Magnox power stations, Proc. WM’01, Tucson, AZ (2001) Paper 52-02.

[4] WSP/100: Introduction to the Nirex Waste Package Specification and Guidance Documentation, Nirex Ltd. Waste Package Specification and Guidance Documentation 481350, July 2005.

[5] SETIADI, A., MILESTONE, N.B., HILL, J., HAYES, M., Corrosion of aluminium and magnesium in BFS composite cements, Adv. Appl. Ceram. 105(4) (2006) 191-196.

[6] SETIADI, A., Corrosion of metals in composite cements. PhD thesis, University of Sheffield, UK (2006).

[7] ZHOU, Q., MILESTONE, N.B., HAYES, M., An alternative to Portland Cement for waste encapsulation-The calcium sulfoaluminate cement system. J. Hazard. Mater. 136 (2006) 120-129.

[8] GIBB, F.G.F., A new scheme for the very deep geological disposal of high level radioactive waste, J. Geol. Soc., London 157 (2000) 27-36.

[9] OJOVAN, M.I., LEE, W.E., An introduction to nuclear waste immobilization. Elsevier, Amsterdam (2005).

[10] OJOVAN, M.I., GIBB, F.G.F., Feasibility of very deep self-disposal for sealed radioactive sources, Proc. WM’05, Tucson, Arizona, WM’05-5072 (2005).

[11] OJOVAN, M.I., GIBB, F.G.F., POLUEKTOV, P.P., EMETS, E.P., Probing of the interior layers of the Earth with self-sinking capsules, Atomic Energy 99 (2) (2005) 556-562.

[12] POLLOCK, A.A., Acoustic emission inspection, Technical Report TR-103-96-12/98. Physical Acoustics Corporation (1989).

Page 13: ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS Sheffield... · ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS L.M. SPASOVA, M.I. OJOVAN Immobilisation Science Laboratory,

13

[13] CHOTARD, T.J., SMITH, A., ROTUREAU, D., FARGEOT, D., GAULT, C., Acoustic emission characterisation of calcium aluminate cement hydration at an early stage, J. Eur. Ceram. Soc. 35 (2003) 387-398.

[14] BELLINGER, F., MAZILLE, H., IDRISSI, H., Use of acoustic emission technique for the early detection of aluminium alloys exfoliation corrosion, NDT&E Int. 35 (2002) 385-392.

[15] ONO, K., Current understanding of mechanisms of acoustic emission, J. Strain Anal. 40(1) Special Issue Paper N1 (2005).

[16] ROQUES, A., et al., Investigation of fatigue crack growth in acrylic bone cement using the acoustic emission technique, Biomaterials 25 (2004) 769-778.

[17] SPASOVA, L.M., OJOVAN, M.I., HAYES, M., GODFREY, H., Acoustic emission monitoring of cementitious wasteforms, Proc. 11th Int. Conf. Envir. Remed. Rad. Waste Manag. ICEM’07. September 2-6, 2007, Oud Sint-Jan Hospital Conference Center, Bruges, Belgium. ICEM07-7049, 8p. ASME (2008).

[18] BELOV, V.Z., ALOY, A.S., Using acoustic emission in quality control of class and ceramics for radioactive waste immobilisation, Mat. Res. Soc. Symp. Proc. 807 (2004) 163-168.

[19] TAM, T., WENG, C.C., A study on acoustic emission characteristics of fly ash cement mortar under compression, Cem. Concr. Res. 24(7) (1994) 1335-1346.

[20] GROSSE, C., FRINK, F., KURZ, J.H., REINHARDT, H.W., Improvements of AE technique uses wavelet algorithms, coherence functions and automatic data analysis, Const. Build. Mater. 18 (2004) 203-213.

[21] SPASOVA, L.M., OJOVAN, M.I., Acoustic emission detection of microcrack formation and development in cementitious wasteforms with immobilised Al, J. Hazard. Mater. 138 (3) (2006) 423-432.

[22] SPASOVA, L.M., OJOVAN, M.I., SCALES, C.R., Acoustic Emission monitoring of aluminium corrosion in cemented-based wasteforms, Adv. Mater. Res. 13-14 (2006) 223-229.

[23] SPASOVA, L.M., OJOVAN, M.I., Frequency Characteristics of Acoustic Emission Signals from Cementitious Wasteforms with Encapsulated Al, Mater. Res. Soc. Symp. Proc., 985, NN10-03, 6p., Warrendale, PA (2007).

[24] SPASOVA, L.M., GIBB, F.G.F., OJOVAN, M.I., Characterisation of partial melting and solidification of granite E93/7 by the acoustic emission technique, Mater. Res. Soc. Symp. Proc. 1107 (2008) 75-82.

[25] PHILIPPIDIS, T.P., AGGELIS, G., Experimental study of wave dispersion and attenuation in concrete, Ultrasonics 43 (2005) 584-595.

[26] UDDIN, F.A.K.M., SHIGEISHI, M., OHTSU, M., Fracture mechanics of corrosion cracking in concrete by acoustic emission, Meccanica 41 (2006) 425-442.

[27] GROSSE, C., FINCK, F., Quantitative evaluation of fracture processes in concrete using signal-based acoustic emission technique, Cem. Concr. Compos. 28 (2006) 330-336.

[28] HALROYD, T., MEISURIA, H., Field experiences in the use of an acoustic emission bridge monitoring system, Structural Faults and Repair, Edinburgh, UK (2006).

[29] KAISER, J., Erkenntnisse und Folgerungen aus der Messung von Gerauschen bei Zugbeanspruchung von Metallischen Werkstiffen, Arch. Eisenhuttenwes. 24 (1-2) (1953) 43-45.

[30] WU, K., CHEN, B., YAO, W., Study of the AE characteristics of fracture process of mortar, concrete and steel-fiber-reinforced concrete beams, Cem. Concr. Res. 30 (2000) 1495-1500.

[31] GROSSE, C., REINHARDT, H., FINCK, F., Signal-based acoustic emission techniques in civil engineering, J. Mater. Civil Eng. 15(3) (2003) 274-279.

[32] ATTRILL, P.G., GIBB, F.G.F., Partial melting and recrystallisation of granite and their application to deep disposal of radioactive waste, Part 1 - Rationale and partial melting. Lithos 67 (2003) 103-117.

[33] ATTRILL, P.G., GIBB, F.G.F., Partial melting and recrystallisation of granite and their application to deep disposal of radioactive waste, Part 2 – Recrystallisaton, Lithos 67 (2003) 119-133.

Page 14: ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS Sheffield... · ACOUSTIC EMISSION MONITORING OF CEMENTITIOUS WASTEFORMS L.M. SPASOVA, M.I. OJOVAN Immobilisation Science Laboratory,

14

[34] OHYA, Y., TAKAHASHI, Y., MURATA, M., NEKAGAWA, Z., Acoustic emission from a porcelain body during cooling, J. Amer. Ceram. Soc. 82 (2) (1999) 445-448.

[35] SPASOVA, L.M., OJOVAN, M.I., SCALES, C.R., Acoustic emission technique applied for monitoring and inspection of cementitious structures encapsulating aluminium, J. Acoustic Emission 25 (2007) 51-68.

[36] SPASOVA, L.M., OJOVAN, M.I., Characterisation of Al corrosion and its impact on the mechanical performance of composite cement wasteforms by the acoustic emission technique, J. Nucl. Mater., 375, 347-358 (2008).

[37] SPASOVA, L.M., OJOVAN, M.I., Acoustic emission characterisation of cementitious wasteforms under three-point bending and compression, Mater. Res. Soc. Symp. Proc. 1124, Warrendale, PA, 8p., Q07-21 (2009).