1-D and 2-D Carbon-Iron Nanohybrids Prepared with Ultrasonic Spray Pyrolysis for Cr (VI) Removal
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1 1-D and 2-D Carbon-Iron Nanohybrids Prepared with Ultrasonic Spray Pyrolysis for Cr (VI) Removal Arvid Masud, John D. Atkinson, and Nirupam Aich Civil, Structural and Environmental Engineering 1
2 Nanomaterial Synthesis, Modification, and Conjugation Physicochemical Property Characterization and Application Nanomaterial Safety for Environment and humans Safer-by-Design Multifunctional Nanomaterials for Environmental Application 2
3 Nanomaterial Synthesis, Modification, and Conjugation Physicochemical Property Characterization and Application Nanomaterial Safety for Environment and humans Safer-by-Design Multifunctional Nanomaterials for Environmental Application Material of Choice: Iron and Graphene or CNT 3
4 Environmental Application of Iron Nanoparticle In 2010, world market for environmental application of nanomaterials was $6 Billion Fe NP (mostly nano zero valent iron, nzvi) is the most used engineered nanomaterial for in-situ soil and groundwater remediation High redox activity & adsorptive capacity enable Fe NPs to remove heavy metal and organic contaminants Pilot scale iron nanoparticle based ground water remediation plant through injection well Applied to 77 pilot & field scale sites worldwide (2014) Applied also in pilot wastewater treatment plants 4
5 Limitations to Reactivity and Need for Solid Supports Fe NPs agglomerate due to van der Waals and magnetic attraction forces, decreasing reactivity and adsorption 1-D carbon nanotube (CNT) and 2-D reduced graphene oxide (rgo) are good solid supports Large accessible specific surface area High electron mobility Mechanical durability High contaminant adsorption nzvi Fe NP 5
6 Limitations to Reactivity and Need for Solid Supports Fe NPs agglomerate due to van der Waals and magnetic attraction forces, decreasing reactivity and adsorption 1-D carbon nanotube (CNT) and 2-D reduced graphene oxide (rgo) are good solid supports Large accessible specific surface area High electron mobility Mechanical durability High contaminant adsorption 6
7 Limitations to Reactivity and Need for Solid Supports Fe NPs agglomerate due to van der Waals and magnetic attraction forces, decreasing reactivity and adsorption 1-D carbon nanotube (CNT) and 2-D reduced graphene oxide (rgo) are good solid supports Large accessible specific surface area High electron mobility Mechanical durability High contaminant adsorption Comparison of Fe-CNT and Fe-rGO Effect of Shape of Carbon Nanomaterials nzvi Fe NP 7
8 Nanomaterial Synthesis, Modification, and Conjugation Physicochemical Property Characterization and Application Nanomaterial Safety for Environment and humans Safer-by-Design Multifunctional Nanomaterials for Environmental Application Process of Choice: Ultrasonic Spray Pyrolysis 8
9 Synthesis of Fe-Carbon Nanohybrids Wet Chemistry based methods are conventional Chemical reduction of iron salts onto oxidized CNT or graphene oxide (GO) Some methods require hazardous reducing agents (hydrazine, benzene) Require extensive reaction time (up to 24 hours) Limited by scalability 9
10 Ultrasonic Spray Pyrolysis (USP) Aerosol based process Fast: reactions happen in matter of seconds Thermal reduction: so No hazardous reagents Continuous, one-step, and Scalable process 10
11 Ultrasonic Spray Pyrolysis (USP) Aerosol based process Fast: reactions happen in matter of seconds Thermal reduction: so No hazardous reagents Continuous, one-step, and Scalable process No study on USP-derived Fe-CNT or Fe-rGO for pollutant removal 11
12 Nanohybrid Types and Relevant Precursors Fe-CNT Fe-rGO Oxidized CNT:FeCl 3.6H 2 O = 1:10 Fe-CNT-R1 Oxidized CNT:FeCl 3.6H 2 O = 1:1 Fe-CNT-R2 Graphene Oxide:FeCl 3.6H 2 O = 1:10 Fe-rGO-R1 Graphene Oxide:FeCl 3.6H 2 O = 1:1 Fe-rGO-R2 Fe NP FeCl 3.6H 2 O 12
13 Fe-CNT Fe-rGO Nanohybrid Types and Relevant Precursors R1: High Fe Content and Low Carbon Content Oxidized CNT:FeCl 3.6H 2 O = 1:10 Fe-CNT-R1 Oxidized CNT:FeCl 3.6H 2 O = 1:1 Fe-CNT-R2 Graphene Oxide:FeCl 3.6H 2 O = 1:10 Fe-rGO-R1 Graphene Oxide:FeCl 3.6H 2 O = 1:1 Fe-rGO-R2 Fe NP FeCl 3.6H 2 O 13
14 High Resolution Transmission Electron Microscopy Image Fe NP Size range: nm 14
15 High Resolution Transmission Electron Microscopy Image Fe-CNT-R1 Size range: nm Fe-CNT-R2 Size range: nm 15
16 High Resolution Transmission Electron Microscopy Image Fe-CNT-R1 Size range: nm CNT gets more bundled in USP Fe-CNT-R2 Size range: nm 16
17 High Resolution Transmission Electron Microscopy Image Fe-rGO-R1 Size range: nm Fe-rGO-R2 Size range: 8-15 nm 17
18 High Resolution Transmission Electron Microscopy Image Fe-rGO-R1 Size range: nm rgo thermally exfoliates and crumples Fe-rGO-R2 Size range: 8-15 nm 18
19 X-ray Diffraction Spectroscopy (XRD) Fe 3 O 4 Fe 0 Fe 2 O 3 Graphite Intensity (a.u.) Fe-rGO-R2 Fe -rgo-r1 Fe NP q (degree) More reduced form of Fe NPs with increase of Carbon content 19
20 Thermogravimetric Analyses Fe-rGO-R1 Fe-rGO-R2 Retained Weight (%) % 18% Temperature ( o C) Estimated CNT in Fe-CNT-R1 13% Estimated CNT in Fe-CNT-R2 33% Estimated rgo in Fe-rGO-R1 18% Estimated rgo in Fe-rGO-R %
21 Heavy Metal Removal: Cr (VI) Adsorption Isotherm USP Product Adsorption Capacity (mg/g) BET Surface area (m 2 /g) Fe-rGO-R Fe-rGO-R Fe-CNT-R Fe-CNT-R Fe NPs 6 8 Increased surface area in nanohybrids aid their higher adsorption Fe-rGO-R2: Highest adsorption due to uniformly dispersed and smallest Fe NPs 21
22 Heavy Metal Removal: Cr (VI) Adsorption Isotherm USP Product Adsorption Capacity (mg/g) BET Surface area (m 2 /g) Fe-rGO-R Fe-rGO-R Fe-CNT-R Fe-CNT-R Fe NPs 6 8 Fe-CNT << Fe-rGO Bundled vs Exfoliated Increased surface area in nanohybrids aid their higher adsorption Fe-rGO-R2: Highest adsorption due to uniformly dispersed and smallest Fe NPs 22
23 Summary and Future Perspective USP-derived Fe-rGO performs better than Fe-CNT for Cr(VI) removal (shape-effect) Tuning of Fe content is critical Influence of environmental parameters (ph, ionic strength) needs to be studied More investigation is needed to clarify the mechanisms of contaminant removal Masud, Atkinson, Aich, J Nanopart Res, Submitted 23
24 Nanomaterial Synthesis, Modification, and Conjugation Physicochemical Property Characterization and Application Nanomaterial Safety for Environment and humans Safer-by-Design Multifunctional Nanomaterials for Environmental Application Nanohybrid Toxicity Fe-rGO Nanohybrid Toxicity to Bronchial Epithelial Cell (BEAS-2B) 24
25 Acknowledgements Dr. John Atkinson (UB CSEE) Yanbin Cui 25
26 Thank You 26
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