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 Lab. (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 = {2018},
month = {9}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 9 works
Citation information provided by
Web of Science
Web of Science
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).
All figures and tables
(10 total)
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Mesostructure-Induced Selectivity in CO 2 Reduction Catalysis
journal, November 2015
- Hall, Anthony Shoji; Yoon, Youngmin; Wuttig, Anna
- Journal of the American Chemical Society, Vol. 137, Issue 47
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Monodispersed PtCo nanoparticles on hexadecyltrimethylammonium bromide treated graphene as an effective oxygen reduction reaction catalyst for proton exchange membrane fuel cells
journal, August 2012
- Nam, Kwan-Woo; Song, Jongchan; Oh, Keun-Hwan
- Carbon, Vol. 50, Issue 10
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Electrochemical CO2 Reduction on Metal Electrodes
book, January 2008
- Hori, Y.; Vayenas, Constantinos G.; White, Ralph E.
- Modern Aspects of Electrochemistry, p. 89-189
Methanol Synthesis and Reverse Water–Gas Shift Kinetics over Cu(110) Model Catalysts: Structural Sensitivity
journal, July 1996
- Yoshihara, Jun; Campbell, Charles T.
- Journal of Catalysis, Vol. 161, Issue 2
Special points for Brillouin-zone integrations
journal, June 1976
- Monkhorst, Hendrik J.; Pack, James D.
- Physical Review B, Vol. 13, Issue 12, p. 5188-5192
Insight into Electrochemical CO 2 Reduction on Surface-Molecule-Mediated Ag Nanoparticles
journal, December 2016
- Kim, Cheonghee; Eom, Taedaehyeong; Jee, Michael Shincheon
- ACS Catalysis, Vol. 7, Issue 1
Electrochemical Reduction of CO 2 at Functionalized Au Electrodes
journal, February 2017
- Fang, Yuxin; Flake, John C.
- Journal of the American Chemical Society, Vol. 139, Issue 9
Dispersion Stability of Single-Walled Carbon Nanotubes Using Nafion in Bisolvent
journal, February 2007
- Lee, Jin-Hyon; Paik, Ungyu; Choi, Jae-Young
- The Journal of Physical Chemistry C, Vol. 111, Issue 6
Ab initio molecular dynamics for open-shell transition metals
journal, November 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 48, Issue 17
The Role of Adsorbed CN and Cl on an Au Electrode for Electrochemical CO 2 Reduction
journal, January 2018
- Cho, Minhyung; Song, Jun Tae; Back, Seoin
- ACS Catalysis, Vol. 8, Issue 2
Nanostructured Materials for Heterogeneous Electrocatalytic CO 2 Reduction and their Related Reaction Mechanisms
journal, July 2017
- Zhang, Lei; Zhao, Zhi-Jian; Gong, Jinlong
- Angewandte Chemie International Edition, Vol. 56, Issue 38
A selective and efficient electrocatalyst for carbon dioxide reduction
journal, January 2014
- Lu, Qi; Rosen, Jonathan; Zhou, Yang
- Nature Communications, Vol. 5, Issue 1
Reactions of synthesis gas
journal, September 1996
- Wender, Irving
- Fuel Processing Technology, Vol. 48, Issue 3
Effect of Chloride Anions on the Synthesis and Enhanced Catalytic Activity of Silver Nanocoral Electrodes for CO 2 Electroreduction
journal, August 2015
- Hsieh, Yu-Chi; Senanayake, Sanjaya D.; Zhang, Yu
- ACS Catalysis, Vol. 5, Issue 9
Active Sites of Au and Ag Nanoparticle Catalysts for CO 2 Electroreduction to CO
journal, August 2015
- Back, Seoin; Yeom, Min Sun; Jung, Yousung
- ACS Catalysis, Vol. 5, Issue 9
In Situ Surface-Enhanced Raman Spectroscopy of the Electrochemical Reduction of Carbon Dioxide on Silver with 3,5-Diamino-1,2,4-Triazole
journal, July 2014
- Schmitt, Kevin G.; Gewirth, Andrew A.
- The Journal of Physical Chemistry C, Vol. 118, Issue 31
Inhomogeneous Electron Gas
journal, November 1964
- Hohenberg, P.; Kohn, W.
- Physical Review, Vol. 136, Issue 3B, p. B864-B871
Electrochemical reduction of CO 2 to synthesis gas with controlled CO/H 2 ratios
journal, January 2017
- Sheng, Wenchao; Kattel, Shyam; Yao, Siyu
- Energy & Environmental Science, Vol. 10, Issue 5
Enhancing CO 2 Electroreduction with the Metal–Oxide Interface
journal, April 2017
- Gao, Dunfeng; Zhang, Yi; Zhou, Zhiwen
- Journal of the American Chemical Society, Vol. 139, Issue 16
Monodisperse Au Nanoparticles for Selective Electrocatalytic Reduction of CO 2 to CO
journal, October 2013
- Zhu, Wenlei; Michalsky, Ronald; Metin, Önder
- Journal of the American Chemical Society, Vol. 135, Issue 45
The emerging era of supramolecular polymeric binders in silicon anodes
journal, January 2018
- Kwon, Tae-woo; Choi, Jang Wook; Coskun, Ali
- Chemical Society Reviews, Vol. 47, Issue 6
The teraton challenge. A review of fixation and transformation of carbon dioxide
journal, January 2010
- Mikkelsen, Mette; Jørgensen, Mikkel; Krebs, Frederik C.
- Energy Environ. Sci., Vol. 3, Issue 1
Active and Selective Conversion of CO 2 to CO on Ultrathin Au Nanowires
journal, November 2014
- Zhu, Wenlei; Zhang, Yin-Jia; Zhang, Hongyi
- Journal of the American Chemical Society, Vol. 136, Issue 46
Theoretical Insight into the Trends that Guide the Electrochemical Reduction of Carbon Dioxide to Formic Acid
journal, December 2015
- Yoo, Jong Suk; Christensen, Rune; Vegge, Tejs
- ChemSusChem, Vol. 9, Issue 4
Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode
journal, November 2004
- Nørskov, J. K.; Rossmeisl, J.; Logadottir, A.
- The Journal of Physical Chemistry B, Vol. 108, Issue 46
Defining a Materials Database for the Design of Copper Binary Alloy Catalysts for Electrochemical CO 2 Conversion
journal, January 2018
- Lee, Chan Woo; Yang, Ki Dong; Nam, Dae-Hyun
- Advanced Materials, Vol. 30, Issue 42
Opportunities and Challenges in Utilizing Metal-Modified Transition Metal Carbides as Low-Cost Electrocatalysts
journal, October 2017
- Tackett, Brian M.; Sheng, Wenchao; Chen, Jingguang G.
- Joule, Vol. 1, Issue 2
Prospects of CO2 Utilization via Direct Heterogeneous Electrochemical Reduction
journal, December 2010
- Whipple, Devin T.; Kenis, Paul J. A.
- The Journal of Physical Chemistry Letters, Vol. 1, Issue 24, p. 3451-3458
Aqueous CO 2 Reduction at Very Low Overpotential on Oxide-Derived Au Nanoparticles
journal, November 2012
- Chen, Yihong; Li, Christina W.; Kanan, Matthew W.
- Journal of the American Chemical Society, Vol. 134, Issue 49
The Functionality of Surface Hydroxy Groups on the Selectivity and Activity of Carbon Dioxide Reduction over Cuprous Oxide in Aqueous Solutions
journal, May 2018
- Yang, Piaoping; Zhao, Zhi-Jian; Chang, Xiaoxia
- Angewandte Chemie International Edition, Vol. 57, Issue 26
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
journal, April 2010
- Grimme, Stefan; Antony, Jens; Ehrlich, Stephan
- The Journal of Chemical Physics, Vol. 132, Issue 15
Achieving Selective and Efficient Electrocatalytic Activity for CO 2 Reduction Using Immobilized Silver Nanoparticles
journal, October 2015
- Kim, Cheonghee; Jeon, Hyo Sang; Eom, Taedaehyeong
- Journal of the American Chemical Society, Vol. 137, Issue 43
Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965
- Kohn, W.; Sham, L. J.
- Physical Review, Vol. 140, Issue 4A, p. A1133-A1138
Tuning the Catalytic Activity and Selectivity of Cu for CO 2 Electroreduction in the Presence of Halides
journal, February 2016
- Varela, Ana Sofia; Ju, Wen; Reier, Tobias
- ACS Catalysis, Vol. 6, Issue 4
Inhomogeneous Electron Gas
journal, March 1973
- Rajagopal, A. K.; Callaway, J.
- Physical Review B, Vol. 7, Issue 5
The Functionality of Surface Hydroxy Groups on the Selectivity and Activity of Carbon Dioxide Reduction over Cuprous Oxide in Aqueous Solutions
journal, May 2018
- Yang, Piaoping; Zhao, Zhi-Jian; Chang, Xiaoxia
- Angewandte Chemie, Vol. 130, Issue 26
High-resolution X-ray luminescence extension imaging
journal, February 2021
- Ou, Xiangyu; Qin, Xian; Huang, Bolong
- Nature, Vol. 590, Issue 7846
Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect
journal, February 2020
- Tatemizo, Nobuyuki; Imada, Saki; Okahara, Kizuna
- Scientific Reports, Vol. 10, Issue 1
Works referencing / citing this record:
Atomic Ni Anchored Covalent Triazine Framework as High Efficient Electrocatalyst for Carbon Dioxide Conversion
journal, March 2019
- Lu, Chenbao; Yang, Jian; Wei, Shice
- Advanced Functional Materials, Vol. 29, Issue 10
Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO 2 by Supporting Palladium on Metal Carbides
journal, February 2019
- Wang, Jiajun; Kattel, Shyam; Hawxhurst, Christopher J.
- Angewandte Chemie, Vol. 131, Issue 19
Kopplung von Solarenergie und Wärmeenergie zur Kohlendioxidreduktion: Aktueller Stand und Perspektiven
journal, February 2020
- Wang, Zhou‐jun; Song, Hui; Liu, Huimin
- Angewandte Chemie, Vol. 132, Issue 21
Electrochemical Conversion of CO 2 to Syngas with Controllable CO/H 2 Ratios over Co and Ni Single‐Atom Catalysts
journal, January 2020
- He, Qun; Liu, Daobin; Lee, Ji Hoon
- Angewandte Chemie, Vol. 132, Issue 8
Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO 2 by Supporting Palladium on Metal Carbides
journal, April 2019
- Wang, Jiajun; Kattel, Shyam; Hawxhurst, Christopher J.
- Angewandte Chemie International Edition, Vol. 58, Issue 19
Coupling of Solar Energy and Thermal Energy for Carbon Dioxide Reduction: Status and Prospects
journal, February 2020
- Wang, Zhou-jun; Song, Hui; Liu, Huimin
- Angewandte Chemie International Edition
Electrochemical Conversion of CO 2 to Syngas with Controllable CO/H 2 Ratios over Co and Ni Single-Atom Catalysts
journal, January 2020
- He, Qun; Liu, Daobin; Lee, Ji Hoon
- Angewandte Chemie International Edition, Vol. 59, Issue 8
Progress in development of electrocatalyst for CO 2 conversion to selective CO production
journal, March 2020
- Nguyen, Dang Le Tri; Kim, Younghye; Hwang, Yun Jeong
- Carbon Energy, Vol. 2, Issue 1
Tuning the activity and selectivity of electroreduction of CO2 to synthesis gas using bimetallic catalysts
journal, August 2019
- Lee, Ji Hoon; Kattel, Shyam; Jiang, Zhao
- Nature Communications, Vol. 10, Issue 1
Isotopic effect on electrochemical CO 2 reduction activity and selectivity in H 2 O- and D 2 O-based electrolytes over palladium
journal, January 2020
- Lee, Ji Hoon; Tackett, Brian M.; Xie, Zhenhua
- Chemical Communications, Vol. 56, Issue 1
Enhanced CO 2 electroreduction performance over Cl-modified metal catalysts
journal, January 2019
- Fu, Huai Qin; Zhang, Le; Zheng, Li Rong
- Journal of Materials Chemistry A, Vol. 7, Issue 20
Understanding the role of functional groups of thiolate ligands in electrochemical CO 2 reduction over Au(111) from first-principles
journal, January 2019
- Li, Fuhua; Tang, Qing
- Journal of Materials Chemistry A, Vol. 7, Issue 34
CO 2 electrolysis to multicarbon products at activities greater than 1 A cm −2
journal, February 2020
- García de Arquer, F. Pelayo; Dinh, Cao-Thang; Ozden, Adnan
- Science, Vol. 367, Issue 6478
Inside Cover: Electrochemical Conversion of CO 2 to Syngas with Controllable CO/H 2 Ratios over Co and Ni Single‐Atom Catalysts (Angew. Chem. Int. Ed. 8/2020)
journal, February 2020
- He, Qun; Liu, Daobin; Lee, Ji Hoon
- Angewandte Chemie International Edition, Vol. 59, Issue 8
Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.