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Title: 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:
 [1];  [1];  [1];  [2]; ORCiD logo [1]; ORCiD logo [3]
+ Show Author Affiliations
  1. Univ. of California, Berkeley, CA (United States). Department of Chemistry
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry
  3. 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.
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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
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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.
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@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}
}
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    • DOI: 10.1002/anie.201909069

    Manganese acting as a high-performance heterogeneous electrocatalyst in carbon dioxide reduction
    journal, July 2019

    Photoactive Earth‐Abundant Iron Pyrite Catalysts for Electrocatalytic Nitrogen Reduction Reaction
    journal, October 2019

    Surface organometallic chemistry in heterogeneous catalysis
    journal, January 2018

    • Samantaray, Manoja K.; Pump, Eva; Bendjeriou-Sedjerari, Anissa
    • Chemical Society Reviews, Vol. 47, Issue 22
    • DOI: 10.1039/c8cs00356d

    Carbon Materials as Cathode Constituents for Electrochemical CO2 Reduction—A Review
    journal, December 2019

    • Messias, Sofia; Nunes da Ponte, Manuel; S. Reis-Machado, Ana
    • C — Journal of Carbon Research, Vol. 5, Issue 4
    • DOI: 10.3390/c5040083

    Recent Advances in Electrochemical CO 2 -to-CO Conversion on Heterogeneous Catalysts
    journal, August 2018

    • Zheng, Tingting; Jiang, Kun; Wang, Haotian
    • Advanced Materials, Vol. 30, Issue 48
    • DOI: 10.1002/adma.201802066

    Achieving Simultaneous CO 2 and H 2 S Conversion via a Coupled Solar-Driven Electrochemical Approach on Non-Precious-Metal Catalysts
    journal, February 2018

    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
    • DOI: 10.1002/cey2.27

    Synergistic Effect of Dual Particle-Size AuNPs on TiO2 for Efficient Photocatalytic Hydrogen Evolution
    journal, April 2019

    Steering post-C–C coupling selectivity enables high efficiency electroreduction of carbon dioxide to multi-carbon alcohols
    journal, June 2018

    Enhancing CO 2 Electroreduction with Au/Pyridine/Carbon Nanotubes Hybrid Structures
    journal, April 2019

    Nanoporous Cu/Ni oxide composites: efficient catalysts for electrochemical reduction of CO 2 in aqueous electrolytes
    journal, January 2018

    • Yang, Dexin; Zhu, Qinggong; Sun, Xiaofu
    • Green Chemistry, Vol. 20, Issue 16
    • DOI: 10.1039/c8gc01552j

    Tuning Gold Nanoparticles with Chelating Ligands for Highly Efficient Electrocatalytic CO 2 Reduction
    journal, August 2018

    • Cao, Zhi; Zacate, Samson B.; Sun, Xiaodong
    • Angewandte Chemie, Vol. 130, Issue 39
    • DOI: 10.1002/ange.201805696

    Microwave-assisted synthesis of AuNPs/CdS composite nanorods for enhanced photocatalytic hydrogen evolution
    journal, January 2019

    Stannate derived bimetallic nanoparticles for electrocatalytic CO 2 reduction
    journal, January 2018

    • Zhang, Xiaolong; Li, Fengwang; Zhang, Ying
    • Journal of Materials Chemistry A, Vol. 6, Issue 17
    • DOI: 10.1039/c8ta02429d

    Insights into in situ one-step synthesis of carbon-supported nano-particulate gold-based catalysts for efficient electrocatalytic CO 2 reduction
    journal, January 2018

    • Zhang, Yicheng; Hu, Liang; Han, Weiqiang
    • Journal of Materials Chemistry A, Vol. 6, Issue 46
    • DOI: 10.1039/c8ta08698b

    A Polymer Solution To Prevent Nanoclustering and Improve the Selectivity of Metal Nanoparticles for Electrocatalytic CO 2 Reduction
    journal, September 2019

    • Zhang, Lei; Wei, Zichao; Thanneeru, Srinivas
    • Angewandte Chemie, Vol. 131, Issue 44
    • DOI: 10.1002/ange.201909069

    Tuning Gold Nanoparticles with Chelating Ligands for Highly Efficient Electrocatalytic CO 2 Reduction
    journal, August 2018

    • Cao, Zhi; Zacate, Samson B.; Sun, Xiaodong
    • Angewandte Chemie International Edition, Vol. 57, Issue 39
    • DOI: 10.1002/anie.201805696
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