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Title: Understanding the Role of Functional Groups in Polymeric Binder for Electrochemical Carbon Dioxide Reduction on Gold Nanoparticles

Abstract

Electrochemical CO 2 reduction reaction (CO 2RR) is one of the promising strategies for converting CO 2 to value-added chemicals. Gold (Au) catalysts are considered to be the best benchmarking materials for CO 2RR to produce CO. In this work, the role of different functional groups of polymeric binders on CO 2RR 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 CO 2RR, thus enabling more catalytic active sites to be available for CO 2RR and enhancing the CO 2RR 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 CO 2RR.

Authors:
ORCiD logo [1];  [2];  [1];  [1];  [3];  [3]; ORCiD logo [4]
  1. Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
  3. Tianjin Univ., Tianjin (China). Collaborative Innovation Center of Chemical Science and Engineering, School of Chemical Engineering and Technology
  4. 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) (SC-22)
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
Resource Type:
Journal Article: 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. doi: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. doi:10.1002/adfm.201804762.
@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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