Synergistic Enhancement of Electrocatalytic CO2 Reduction with Gold Nanoparticles Embedded in Functional Graphene Nanoribbon Composite Electrodes
Abstract
Regulating the complex environment accounting for the stability, selectivity, and activity of catalytic metal nanoparticle interfaces represents a challenge to heterogeneous catalyst design. Here in this paper, we demonstrate the intrinsic performance enhancement of a composite material composed of gold nanoparticles (AuNPs) embedded in a bottom-up synthesized graphene nanoribbon (GNR) matrix for the electrocatalytic reduction of CO2. Electrochemical studies reveal that the structural and electronic properties of the GNR composite matrix increase the AuNP electrochemically active surface area (ECSA), lower the requisite CO2 reduction overpotential by hundreds of millivolts (catalytic onset > -0.2 V versus reversible hydrogen electrode (RHE)), increase the Faraday efficiency (>90%), markedly improve stability (catalytic performance sustained over >24 h), and increase the total catalytic output (>100-fold improvement over traditional amorphous carbon AuNP supports). The inherent structural and electronic tunability of bottom-up synthesized GNR-AuNP composites affords an unrivaled degree of control over the catalytic environment, providing a means for such profound effects as shifting the rate-determining step in the electrocatalytic reduction of CO2 to CO, and thereby altering the electrocatalytic mechanism at the nanoparticle surface.
- Authors:
-
- Univ. of California, Berkeley, CA (United States). Department of Chemistry
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry
- Univ. of California, Berkeley, CA (United States). Department of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Material Sciences Division; Kavli Energy Nanosciences Institute at the University of California Berkeley and Lawrence Berkeley National Laboratory, Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1437957
- Grant/Contract Number:
- AC02-05CH11231; SC0010409
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 139; Journal Issue: 11; Related Information: © 2017 American Chemical Society.; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE
Citation Formats
Rogers, Cameron, Perkins, Wade S., Veber, Gregory, Williams, Teresa E., Cloke, Ryan R., and Fischer, Felix R. Synergistic Enhancement of Electrocatalytic CO2 Reduction with Gold Nanoparticles Embedded in Functional Graphene Nanoribbon Composite Electrodes. United States: N. p., 2017.
Web. doi:10.1021/jacs.6b12217.
Rogers, Cameron, Perkins, Wade S., Veber, Gregory, Williams, Teresa E., Cloke, Ryan R., & Fischer, Felix R. Synergistic Enhancement of Electrocatalytic CO2 Reduction with Gold Nanoparticles Embedded in Functional Graphene Nanoribbon Composite Electrodes. United States. https://doi.org/10.1021/jacs.6b12217
Rogers, Cameron, Perkins, Wade S., Veber, Gregory, Williams, Teresa E., Cloke, Ryan R., and Fischer, Felix R. Fri .
"Synergistic Enhancement of Electrocatalytic CO2 Reduction with Gold Nanoparticles Embedded in Functional Graphene Nanoribbon Composite Electrodes". United States. https://doi.org/10.1021/jacs.6b12217. https://www.osti.gov/servlets/purl/1437957.
@article{osti_1437957,
title = {Synergistic Enhancement of Electrocatalytic CO2 Reduction with Gold Nanoparticles Embedded in Functional Graphene Nanoribbon Composite Electrodes},
author = {Rogers, Cameron and Perkins, Wade S. and Veber, Gregory and Williams, Teresa E. and Cloke, Ryan R. and Fischer, Felix R.},
abstractNote = {Regulating the complex environment accounting for the stability, selectivity, and activity of catalytic metal nanoparticle interfaces represents a challenge to heterogeneous catalyst design. Here in this paper, we demonstrate the intrinsic performance enhancement of a composite material composed of gold nanoparticles (AuNPs) embedded in a bottom-up synthesized graphene nanoribbon (GNR) matrix for the electrocatalytic reduction of CO2. Electrochemical studies reveal that the structural and electronic properties of the GNR composite matrix increase the AuNP electrochemically active surface area (ECSA), lower the requisite CO2 reduction overpotential by hundreds of millivolts (catalytic onset > -0.2 V versus reversible hydrogen electrode (RHE)), increase the Faraday efficiency (>90%), markedly improve stability (catalytic performance sustained over >24 h), and increase the total catalytic output (>100-fold improvement over traditional amorphous carbon AuNP supports). The inherent structural and electronic tunability of bottom-up synthesized GNR-AuNP composites affords an unrivaled degree of control over the catalytic environment, providing a means for such profound effects as shifting the rate-determining step in the electrocatalytic reduction of CO2 to CO, and thereby altering the electrocatalytic mechanism at the nanoparticle surface.},
doi = {10.1021/jacs.6b12217},
journal = {Journal of the American Chemical Society},
number = 11,
volume = 139,
place = {United States},
year = {Fri Feb 24 00:00:00 EST 2017},
month = {Fri Feb 24 00:00:00 EST 2017}
}
Web of Science
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Achieving Simultaneous CO 2 and H 2 S Conversion via a Coupled Solar-Driven Electrochemical Approach on Non-Precious-Metal Catalysts
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