Nanomaterials Nanomaterials Characterization for Characterization for Studying Environmental Fate Studying Environmental Fate and Transport and Transport Joel A. Pedersen Joel A. Pedersen Environmental Chemistry and Environmental Chemistry and Technology Program Technology Program University of Wisconsin – Madison University of Wisconsin – Madison
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Nanomaterials Characterization for Studying Environmental Fate and Transport Joel A. Pedersen Environmental Chemistry and Technology Program University.
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Nanomaterials Nanomaterials Characterization for Characterization for
Studying Environmental Fate Studying Environmental Fate and Transportand Transport
Joel A. PedersenJoel A. Pedersen
Environmental Chemistry and Technology Environmental Chemistry and Technology ProgramProgram
University of Wisconsin – MadisonUniversity of Wisconsin – Madison
Subsurface Transport and Subsurface Transport and FateFate
Fin
lays
on
-Pitt
s a
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Pitt
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98
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Chemical CompositionChemical Composition Bulk chemical compositionBulk chemical composition
Elemental analysis, ICP-MS, energy-dispersive X-ray Elemental analysis, ICP-MS, energy-dispersive X-ray analysis (EDX), electron energy loss spectroscopy (EELS), analysis (EDX), electron energy loss spectroscopy (EELS), dynamic secondary ion mass spectrometry (SIMS), atom-dynamic secondary ion mass spectrometry (SIMS), atom-probe tomographyprobe tomography
Surface chemical composition Surface chemical composition X-ray photoelectron (XPS), Auger, FTIR, Raman and surface X-ray photoelectron (XPS), Auger, FTIR, Raman and surface
Nature and length of attached moleculeNature and length of attached molecule Functionalization densityFunctionalization density
Thermogravimetic analysis (TGA) + BET Thermogravimetic analysis (TGA) + BET [Marcinko and Fadeev, 2004][Marcinko and Fadeev, 2004]; XPS; XPS
Type of attachmentType of attachment Anchoring group (covalently grafted) Anchoring group (covalently grafted) Mechanism (e.g., adsorption, covalent)Mechanism (e.g., adsorption, covalent)
FTIR, XPSFTIR, XPS
Nanoparticle SizeNanoparticle Size Primary particle size distributionPrimary particle size distribution
SEM, TEMSEM, TEM Hydrodynamic size distributionHydrodynamic size distribution
Hard sphere that diffuses with the same speed Hard sphere that diffuses with the same speed as the particle under examinationas the particle under examination
DLSDLS
Aerodynamic size distributionAerodynamic size distribution Sphere of unit density with same settling velocitySphere of unit density with same settling velocity Moody impactor, differential mobility analyzer, Moody impactor, differential mobility analyzer,
Polar or Lewis acid-base (AB) interactionsPolar or Lewis acid-base (AB) interactions LWLW, , ABAB , , , , [van Oss, 2006] [van Oss, 2006]
Steric interactionsSteric interactions Functionalization density, radius of gyration [Butt et al., Functionalization density, radius of gyration [Butt et al.,
2007]2007] Surface roughness Surface roughness [Bhattacharjee et al., 1998][Bhattacharjee et al., 1998]
Asperity size, asperity densityAsperity size, asperity density Aggregation/agglomeration stateAggregation/agglomeration state
Aggregation kineticsAggregation kinetics Critical coagulation concentration depends on Critical coagulation concentration depends on
electrolyte concentration and valenceelectrolyte concentration and valence [Chen and [Chen and Elimelech, 2006; Brant et al., 2007]Elimelech, 2006; Brant et al., 2007]
Change in Surface Chemistry: Change in Surface Chemistry: Acquisition of CoatingsAcquisition of Coatings
Amorphous mineral coatings Amorphous mineral coatings Humic substancesHumic substances [Hyung et al., 2007] [Hyung et al., 2007]
Organic compounds condensing on Organic compounds condensing on airborne nanoparticlesairborne nanoparticles
dissolution kinetics as dissolution kinetics as function of pH, function of pH, EEHH, , other constituentsother constituents
Effects of roughness, Effects of roughness, porosity, lattice porosity, lattice defects defects [Yerba et al., 2006][Yerba et al., 2006]
Ruby et al. (1999)
Size-dependent Size-dependent EEHH00 (ZnO) (ZnO)
Hoyer and Weller (1994)
• Semiconductors – in quantum confinement regime Semiconductors – in quantum confinement regime [Brus, 1983; Rossetti et al., 1983; Hoyer and Weller, 1994][Brus, 1983; Rossetti et al., 1983; Hoyer and Weller, 1994]• Metals – Metals – EEHH
00 increases with nuclearity up to metal- increases with nuclearity up to metal-like phase (e.g., for Ag, like phase (e.g., for Ag, ddpp < 1.2 nm ( < 1.2 nm (nn = 80-100)) = 80-100)) [Belloni, 1996][Belloni, 1996]
Surface chemical modificationsSurface chemical modifications Hydroxylation of nCHydroxylation of nC6060 fullerenes fullerenes [Brant et al., [Brant et al.,
2007]2007]
Photocorrosion (semiconductors)Photocorrosion (semiconductors) Alterations in coatingsAlterations in coatings
Biomodification of Surface Biomodification of Surface CoatingsCoatings
Daphnia magna Daphnia magna ingest ingest lysophophatidylcholine-coated SWCNTslysophophatidylcholine-coated SWCNTs
Coating removed and metabolizedCoating removed and metabolized Naked, insoluble CNTs excreted (confirmed Naked, insoluble CNTs excreted (confirmed
by Raman)by Raman)Roberts et al., 2007
Measurement Challenges Measurement Challenges
Detection of NPs in environmental Detection of NPs in environmental matricesmatrices Model, more easily tracked compoundsModel, more easily tracked compounds Radiolabeled materials Radiolabeled materials [Petersen et al., 2006][Petersen et al., 2006]
Sorption of common organic (e.g., PAHs) Sorption of common organic (e.g., PAHs) and inorganic contaminants (e.g., metals) and inorganic contaminants (e.g., metals) [Yang and Xing, 2006][Yang and Xing, 2006]
Reactions with environmental Reactions with environmental contaminants and organic mattercontaminants and organic matter Materials that are active in the UV – mediate Materials that are active in the UV – mediate
reactions on surface of airborne NPs? reactions on surface of airborne NPs? Surface defects – influence adsorption, Surface defects – influence adsorption,
nucleation, surface reactions nucleation, surface reactions [Belon and Epron, 2005; [Belon and Epron, 2005; Butt et al., 2006]Butt et al., 2006]
Chemical compositionChemical composition Particle size and morphologyParticle size and morphology Specific surface areaSpecific surface area Surface charge/potential as Surface charge/potential as ff(pH)(pH) Surface energiesSurface energies Agglomeration stateAgglomeration state Reactive surface area, ROS production, Reactive surface area, ROS production,
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Energy Balance DiagramEnergy Balance Diagram
van Oss (2006)
Variability in Variability in KKococ and and KKd,solidd,solid
Adapted from Tolls (2001), Thiele (200) and Loke et al. (2002)
log log KKdomdom vs. Hydrophobicity vs. Hydrophobicity