Fate, Transport, and Transformation of Carbonaceous Nanomaterials: Progress and Data Gaps
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1 Fate, Transport, and Transformation of Carbonaceous Nanomaterials: Progress and Data Gaps Navid Saleh Civil and Environmental Engineering University of South Carolina tel: (O) 1
2 Allotropes of Carbon C 60 Fullerene Kroto et al.,1985 SWNT Graphene MWNT Clear images of CNTs by Iijima (discovery of MWNTs), 1991
3 Conjugation Lead to Nanohybrids 3
4 Trends in Research & Commercialization De Volder et al. Science. 2013, 339, (6119), Saleh et al. Environ Sci Technol (in review)
5 Environmentally Important Properties A wide range of van der Waals energetics function of size, atomic orientation influence Surface potential high electron affinity Surface activity adsorbing tendency, ligand exchange ability, non-specific short-ranged interaction Reactive surfaces produces ROS, are functionalized with numerous groups 5
6 Importance of Fate and Transport
7 Carbonaceous NMs Aggregation, Deposition, and Transformation Studies
8 Progress Thus Far: Aggregation -synthesis method (Wiesner, Vikesland) -derivatives and surface groups (Isaacson, Jae-Hong Kim) -NOM (Baoshan Xing, Bouchard, Elimelech) -solute condition, background chemistry -Oxidation state (Fairbrother) -surfactants/lipids/biomolecules (Bouchard, Elimelech, Zhang, Nel) -NOM (C.P. Huang, Saleh) -chirality (Saleh) -solute condition, background chemistry -Graphene oxides, NOM (Bouchard) 8
9 Progress Thus Far: Deposition/Transport -background chemistry (Elimelech, Wiesner, Pennell) -humic Acid/surfactant/biofilm (Wiesner, Qilin Li) -systems parameters (Bouchard, Abriola, Pennell) -Synthesis methods (Walker) -surface properties/surfactants (Gao, Huang) -NOM (Saleh) -tube length (Pennell, Peterson) -systems parameters (Elimelech) -Graphene oxides (Walker, Xu, ) -systems parameters (Gao) 9
10 Progress Thus Far: Transformation -photo-transformation (Jae-Hong Kim,Zepp, Qilin Li, Wiesner, Bouchard) -ambient env chemicals (Vikesland, ) -NOM (Baoshan Xing, Alvarez, Qilin Li, Zepp) -photoreactivity (Jafvert) -chemical transformation (Baltog) -thermal transformation (Falaras) -Bacterial transformation (James Tour) 10
11 Fate, Transport, and Transformation: Data Gaps Clean System NP (Individual vs. aggregates) travel and deposition to sediment bed Coexistence of other particles Presence of humics, proteins, surfactants, enzymes Simultaneous coating exchange and heteroaggregation Surface water MATERIAL ATTRIBUTE SYSTEMS ATTRIBUTE 11
12 DOES MATERIAL ATTRIBUTE MATTER? 12
13 Attachment Efficiency CCC(M of NaCl) Higher Fullerenes C 60 C 70 C C 60 C 70 C Equatio y = a Adj. R-S Value Standard B Interc B Slope NaCl Concentration, M Electron Affinity, (ev)
14 Chirality and SWNTs Attachment Efficiency, (a) SG65 SG NaCl Concentration (M) Sample mm NaCl mm CaCl 2 SG SG Metallic Semi-conductive Chiral Nanotubes (Hersam, 2008) 14
15 Nanohybrid for Fuel Cells 100 nm Pt L α1 Ti K α1 Nb 15 K α1
16 Nanohybrid for Fuel Cells Attachment Efficiency, NaCl Concentration, M OMCNT OMCNT-TiO 2 OMCNT-TiO 2 -Pt OMCNT-TiNbO 2 OMCNT-TiNbO 2 -Pt
17 DO SYSTEMS PARAMETERS MATTER? 17
18 Hetero-aggregation (a) (b) PA-SWNT PA-SWNT 100 nm 100 nm 18
19 Co-transport 1.0 Tracer nito nito+swnt C/C Flow Direction Pore Volume SEM Sample Collection Region 19
20 Co-transport Mechanisms Control Collector nito Only nito Co-Transport
21 Co-transport 21
22 SWNT Transport in Solid Waste-Relevant Conditions Mixed MSW and individual media [HA]= 400, 200, 50, and 10 mg TOC/L [AA]= 400 mg TOC/L 200 mm NaCl CO 2 saturated Water saturated HA saturated After SWNT run 22
23 Transport: Individual Collector Type Paper C/C A B Tracer 50 mg/l HA Pore Volume C (a) Paper Glass C/C A B (b) Glass Tracer 50 mg/l HA Pore Volume C A B C (c) Metal Tracer 50 mg/l HA A B C (d) Plastics Tracer 50 mg/l HA C/C C/C Metal Pore Volume Plastics Pore Volume Porous Media % Recovery Paper 20 Glass 93 Metal 77 Plastic 88
24 Research Opportunities Materials Perspective: Perform fate and transport studies on materials from simulated release: solid state vs. polymer composite etc. Higher Fullerenes: identify specific higher fullerene of environmental importance CNTs: develop guidance for chiral-specific SWNTs; effect of length on deposition; improve theoretical models for mechanistic understanding Hybrids: develop strategies for improving choice of hybrid combinations; evaluate hybrid stability during transport and transformation Use MD simulation for material choice and hypothesis development Systems Perspective: Study hetero systems and identify mechanisms of aggregation and deposition; develop prediction models for multi-particle systems Evaluate geo- and bio-macromolecule exchange with synthetic coatings Determine fate and transport in complex environment (landfills, surface water with complex composition) Study the role of synthetic organics on nanomaterial fate and transport Develop adaptive prediction models for fate and transport of transformed nanomaterials
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