Understanding the Role of Functional Groups in Polymeric Binder for Electrochemical Carbon Dioxide Reduction on Gold Nanoparticles
Abstract
Electrochemical CO2 reduction reaction (CO2RR) is one of the promising strategies for converting CO2 to value-added chemicals. Gold (Au) catalysts are considered to be the best benchmarking materials for CO2RR to produce CO. In this work, the role of different functional groups of polymeric binders on CO2RR over Au catalysts is systematically investigated by combined experimental measurements and density functional theory (DFT) calculations. Especially, it is revealed that the functional groups can play a role in suppressing the undesired hydrogen evolution reaction, the main competing reaction against CO2RR, thus enabling more catalytic active sites to be available for CO2RR and enhancing the CO2RR activity. Consistent with the DFT prediction, fluorine (F)-containing functional groups in the F-rich polytetrafluoroethylene binder lead to a high Faradaic efficiency (≈94.7%) of CO production. Finally, this study suggests a new strategy by optimizing polymeric binders for the selective CO2RR.
- Authors:
-
[1];
[4]
- Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
- Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
- Tianjin Univ., Tianjin (China). Collaborative Innovation Center of Chemical Science and Engineering, School of Chemical Engineering and Technology
- Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1484884
- Alternate Identifier(s):
- OSTI ID: 1472160
- Report Number(s):
- BNL-209654-2018-JAAM
Journal ID: ISSN 1616-301X
- Grant/Contract Number:
- SC0012704; FG02-13ER16381; SC0009476
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Functional Materials
- Additional Journal Information:
- Journal Volume: 28; Journal Issue: 45; Journal ID: ISSN 1616-301X
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; electrochemical carbon dioxide reduction; functional groups; binders; density functional theories; gold
Citation Formats
Lee, Ji Hoon, Kattel, Shyam, Xie, Zhenhua, Tackett, Brian M., Wang, Jiajun, Liu, Chang-Jun, and Chen, Jingguang G. Understanding the Role of Functional Groups in Polymeric Binder for Electrochemical Carbon Dioxide Reduction on Gold Nanoparticles. United States: N. p., 2018.
Web. doi:10.1002/adfm.201804762.
Lee, Ji Hoon, Kattel, Shyam, Xie, Zhenhua, Tackett, Brian M., Wang, Jiajun, Liu, Chang-Jun, & Chen, Jingguang G. Understanding the Role of Functional Groups in Polymeric Binder for Electrochemical Carbon Dioxide Reduction on Gold Nanoparticles. United States. https://doi.org/10.1002/adfm.201804762
Lee, Ji Hoon, Kattel, Shyam, Xie, Zhenhua, Tackett, Brian M., Wang, Jiajun, Liu, Chang-Jun, and Chen, Jingguang G. Wed .
"Understanding the Role of Functional Groups in Polymeric Binder for Electrochemical Carbon Dioxide Reduction on Gold Nanoparticles". United States. https://doi.org/10.1002/adfm.201804762. https://www.osti.gov/servlets/purl/1484884.
@article{osti_1484884,
title = {Understanding the Role of Functional Groups in Polymeric Binder for Electrochemical Carbon Dioxide Reduction on Gold Nanoparticles},
author = {Lee, Ji Hoon and Kattel, Shyam and Xie, Zhenhua and Tackett, Brian M. and Wang, Jiajun and Liu, Chang-Jun and Chen, Jingguang G.},
abstractNote = {Electrochemical CO2 reduction reaction (CO2RR) is one of the promising strategies for converting CO2 to value-added chemicals. Gold (Au) catalysts are considered to be the best benchmarking materials for CO2RR to produce CO. In this work, the role of different functional groups of polymeric binders on CO2RR over Au catalysts is systematically investigated by combined experimental measurements and density functional theory (DFT) calculations. Especially, it is revealed that the functional groups can play a role in suppressing the undesired hydrogen evolution reaction, the main competing reaction against CO2RR, thus enabling more catalytic active sites to be available for CO2RR and enhancing the CO2RR activity. Consistent with the DFT prediction, fluorine (F)-containing functional groups in the F-rich polytetrafluoroethylene binder lead to a high Faradaic efficiency (≈94.7%) of CO production. Finally, this study suggests a new strategy by optimizing polymeric binders for the selective CO2RR.},
doi = {10.1002/adfm.201804762},
journal = {Advanced Functional Materials},
number = 45,
volume = 28,
place = {United States},
year = {Wed Sep 19 00:00:00 EDT 2018},
month = {Wed Sep 19 00:00:00 EDT 2018}
}
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Figures / Tables:
Figure 1: The chemical structure of the binders used in this study. (A) Nafion, (B) polyvinyl alcohol (PVA), (C) polyacrylic acid (PAA), (D) polyvinylidene difluoride (PVDF), and (E) polytetrafluoroethylene (PTFE).
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