Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

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

Journal Article · · Advanced Functional Materials
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
+ Show Author Affiliations

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.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012704; FG02-13ER16381; SC0009476
OSTI ID:
1484884
Alternate ID(s):
OSTI ID: 1472160
Report Number(s):
BNL-209654-2018-JAAM
Journal Information:
Advanced Functional Materials, Vol. 28, Issue 45; ISSN 1616-301X
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 70 works
Citation information provided by
Web of Science

References (40)

Mesostructure-Induced Selectivity in CO 2 Reduction Catalysis journal November 2015
Generalized Gradient Approximation Made Simple journal October 1996
Projector augmented-wave method journal December 1994
Monodispersed PtCo nanoparticles on hexadecyltrimethylammonium bromide treated graphene as an effective oxygen reduction reaction catalyst for proton exchange membrane fuel cells journal August 2012
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal July 1996
Electrochemical CO2 Reduction on Metal Electrodes book January 2008
Methanol Synthesis and Reverse Water–Gas Shift Kinetics over Cu(110) Model Catalysts: Structural Sensitivity journal July 1996
Special points for Brillouin-zone integrations journal June 1976
Insight into Electrochemical CO 2 Reduction on Surface-Molecule-Mediated Ag Nanoparticles journal December 2016
Electrochemical Reduction of CO 2 at Functionalized Au Electrodes journal February 2017
Dispersion Stability of Single-Walled Carbon Nanotubes Using Nafion in Bisolvent journal February 2007
Ab initio molecular dynamics for open-shell transition metals journal November 1993
The Role of Adsorbed CN and Cl on an Au Electrode for Electrochemical CO 2 Reduction journal January 2018
Nanostructured Materials for Heterogeneous Electrocatalytic CO 2 Reduction and their Related Reaction Mechanisms journal July 2017
A selective and efficient electrocatalyst for carbon dioxide reduction journal January 2014
Reactions of synthesis gas journal September 1996
Effect of Chloride Anions on the Synthesis and Enhanced Catalytic Activity of Silver Nanocoral Electrodes for CO 2 Electroreduction journal August 2015
Active Sites of Au and Ag Nanoparticle Catalysts for CO 2 Electroreduction to CO journal August 2015
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
Inhomogeneous Electron Gas journal November 1964
Electrochemical reduction of CO 2 to synthesis gas with controlled CO/H 2 ratios journal January 2017
Enhancing CO 2 Electroreduction with the Metal–Oxide Interface journal April 2017
Monodisperse Au Nanoparticles for Selective Electrocatalytic Reduction of CO 2 to CO journal October 2013
The emerging era of supramolecular polymeric binders in silicon anodes journal January 2018
The teraton challenge. A review of fixation and transformation of carbon dioxide journal January 2010
Active and Selective Conversion of CO 2 to CO on Ultrathin Au Nanowires journal November 2014
Theoretical Insight into the Trends that Guide the Electrochemical Reduction of Carbon Dioxide to Formic Acid journal December 2015
Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode journal November 2004
Defining a Materials Database for the Design of Copper Binary Alloy Catalysts for Electrochemical CO 2 Conversion journal January 2018
Opportunities and Challenges in Utilizing Metal-Modified Transition Metal Carbides as Low-Cost Electrocatalysts journal October 2017
Prospects of CO2 Utilization via Direct Heterogeneous Electrochemical Reduction journal December 2010
Aqueous CO 2 Reduction at Very Low Overpotential on Oxide-Derived Au Nanoparticles journal November 2012
The Functionality of Surface Hydroxy Groups on the Selectivity and Activity of Carbon Dioxide Reduction over Cuprous Oxide in Aqueous Solutions journal May 2018
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu journal April 2010
Achieving Selective and Efficient Electrocatalytic Activity for CO 2 Reduction Using Immobilized Silver Nanoparticles journal October 2015
Self-Consistent Equations Including Exchange and Correlation Effects journal November 1965
Tuning the Catalytic Activity and Selectivity of Cu for CO 2 Electroreduction in the Presence of Halides journal February 2016
The Functionality of Surface Hydroxy Groups on the Selectivity and Activity of Carbon Dioxide Reduction over Cuprous Oxide in Aqueous Solutions journal May 2018
High-resolution X-ray luminescence extension imaging journal February 2021
Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect journal February 2020

Cited By (15)

Atomic Ni Anchored Covalent Triazine Framework as High Efficient Electrocatalyst for Carbon Dioxide Conversion journal March 2019
Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO 2 by Supporting Palladium on Metal Carbides journal February 2019
Kopplung von Solarenergie und Wärmeenergie zur Kohlendioxidreduktion: Aktueller Stand und Perspektiven journal February 2020
Electrochemical Conversion of CO 2 to Syngas with Controllable CO/H 2 Ratios over Co and Ni Single‐Atom Catalysts journal January 2020
Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO 2 by Supporting Palladium on Metal Carbides journal April 2019
Coupling of Solar Energy and Thermal Energy for Carbon Dioxide Reduction: Status and Prospects journal February 2020
Electrochemical Conversion of CO 2 to Syngas with Controllable CO/H 2 Ratios over Co and Ni Single-Atom Catalysts journal January 2020
Progress in development of electrocatalyst for CO 2 conversion to selective CO production journal March 2020
Tuning the activity and selectivity of electroreduction of CO2 to synthesis gas using bimetallic catalysts journal August 2019
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
Enhanced CO 2 electroreduction performance over Cl-modified metal catalysts journal January 2019
Understanding the role of functional groups of thiolate ligands in electrochemical CO 2 reduction over Au(111) from first-principles journal January 2019
CO 2 electrolysis to multicarbon products at activities greater than 1 A cm −2 journal February 2020
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
Tuning the activity and selectivity of electroreduction of CO2 to synthesis gas using bimetallic catalysts journal August 2019

Figures / Tables (10)

Figure 1(p. 16)figure Figure 1
Figure 2(p. 17)figure Figure 2
Figure 3(p. 18)figure Figure 3
Figure S1(p. 21)figure Figure S1
Figure S3(p. 21)figure Figure S3
Figure S2(p. 22)figure Figure S2
Figure S4(p. 24)figure Figure S4
Table S1(p. 25)table Table S1
Table S2(p. 26)table Table S2
Table S3(p. 27)table Table S3

Similar Records

Related Subjects

37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
electrochemical carbon dioxide reduction
functional groups
binders
density functional theories
gold