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Title: Electrochemical CO2 Reduction over Compressively Strained CuAg Surface Alloys with Enhanced Multi-Carbon Oxygenate Selectivity

Abstract

The electrochemical reduction of carbon dioxide using renewably generated electricity offers a potential means for producing fuels and chemicals in a sustainable manner. To date, copper has been found to be the most effective catalyst for electrochemically reducing carbon dioxide to products such as methane, ethene, and ethanol. Unfortunately, the current efficiency of the process is limited by competition with the relatively facile hydrogen evolution reaction. Since multi-carbon products are more valuable precursors to chemicals and fuels than methane, there is considerable interest in modifying copper to enhance the multi-carbon product selectivity. In this paper, we report our investigations of electrochemical carbon dioxide reduction over CuAg bimetallic electrodes and surface alloys, which we find to be more selective for the formation of multi-carbon products than pure copper. This selectivity enhancement is a result of the selective suppression of hydrogen evolution, which occurs due to compressive strain induced by the formation of a CuAg surface alloy. Furthermore, we report that these bimetallic electrocatalysts exhibit an unusually high selectivity for the formation of multi-carbon carbonyl-containing products, which we hypothesize to be the consequence of a reduced coverage of adsorbed hydrogen and the reduced oxophilicity of the compressively strained copper. Thus and finally,more » we show that promoting copper surface with small amounts of Ag is a promising means for improving the multi-carbon oxygenated product selectivity of copper during electrochemical CO2 reduction.« less

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1463311
Alternate Identifier(s):
OSTI ID: 1436343
Grant/Contract Number:  
AC02-76SF00515; SC0004993; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 44; 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

Citation Formats

Clark, Ezra L., Hahn, Christopher, Jaramillo, Thomas F., and Bell, Alexis T. Electrochemical CO2 Reduction over Compressively Strained CuAg Surface Alloys with Enhanced Multi-Carbon Oxygenate Selectivity. United States: N. p., 2017. Web. doi:10.1021/jacs.7b08607.
Clark, Ezra L., Hahn, Christopher, Jaramillo, Thomas F., & Bell, Alexis T. Electrochemical CO2 Reduction over Compressively Strained CuAg Surface Alloys with Enhanced Multi-Carbon Oxygenate Selectivity. United States. https://doi.org/10.1021/jacs.7b08607
Clark, Ezra L., Hahn, Christopher, Jaramillo, Thomas F., and Bell, Alexis T. Sat . "Electrochemical CO2 Reduction over Compressively Strained CuAg Surface Alloys with Enhanced Multi-Carbon Oxygenate Selectivity". United States. https://doi.org/10.1021/jacs.7b08607. https://www.osti.gov/servlets/purl/1463311.
@article{osti_1463311,
title = {Electrochemical CO2 Reduction over Compressively Strained CuAg Surface Alloys with Enhanced Multi-Carbon Oxygenate Selectivity},
author = {Clark, Ezra L. and Hahn, Christopher and Jaramillo, Thomas F. and Bell, Alexis T.},
abstractNote = {The electrochemical reduction of carbon dioxide using renewably generated electricity offers a potential means for producing fuels and chemicals in a sustainable manner. To date, copper has been found to be the most effective catalyst for electrochemically reducing carbon dioxide to products such as methane, ethene, and ethanol. Unfortunately, the current efficiency of the process is limited by competition with the relatively facile hydrogen evolution reaction. Since multi-carbon products are more valuable precursors to chemicals and fuels than methane, there is considerable interest in modifying copper to enhance the multi-carbon product selectivity. In this paper, we report our investigations of electrochemical carbon dioxide reduction over CuAg bimetallic electrodes and surface alloys, which we find to be more selective for the formation of multi-carbon products than pure copper. This selectivity enhancement is a result of the selective suppression of hydrogen evolution, which occurs due to compressive strain induced by the formation of a CuAg surface alloy. Furthermore, we report that these bimetallic electrocatalysts exhibit an unusually high selectivity for the formation of multi-carbon carbonyl-containing products, which we hypothesize to be the consequence of a reduced coverage of adsorbed hydrogen and the reduced oxophilicity of the compressively strained copper. Thus and finally, we show that promoting copper surface with small amounts of Ag is a promising means for improving the multi-carbon oxygenated product selectivity of copper during electrochemical CO2 reduction.},
doi = {10.1021/jacs.7b08607},
journal = {Journal of the American Chemical Society},
number = 44,
volume = 139,
place = {United States},
year = {2017},
month = {10}
}

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  • DOI: 10.1039/c8ee01501e

Selective reduction of CO to acetaldehyde with CuAg electrocatalysts
journal, January 2020

  • Wang, Lei; Higgins, Drew C.; Ji, Yongfei
  • Proceedings of the National Academy of Sciences, Vol. 117, Issue 23
  • DOI: 10.1073/pnas.1821683117

Electroreduction of CO 2 on Single‐Site Copper‐Nitrogen‐Doped Carbon Material: Selective Formation of Ethanol and Reversible Restructuration of the Metal Sites
journal, September 2019

  • Karapinar, Dilan; Huan, Ngoc Tran; Ranjbar Sahraie, Nastaran
  • Angewandte Chemie, Vol. 131, Issue 42
  • DOI: 10.1002/ange.201907994

Efficient electrocatalytic CO2 reduction on a three-phase interface
journal, July 2018


Rational Design of Ag‐Based Catalysts for the Electrochemical CO 2 Reduction to CO: A Review
journal, December 2019


Hydroxide promotes carbon dioxide electroreduction to ethanol on copper via tuning of adsorbed hydrogen
journal, December 2019


Optimizing Electron Densities of Ni‐N‐C Complexes by Hybrid Coordination for Efficient Electrocatalytic CO 2 Reduction
journal, February 2020


Current progress of metallic and carbon-based nanostructure catalysts towards the electrochemical reduction of CO 2
journal, January 2019

  • Hou, Liang; Yan, Jingze; Takele, Leta
  • Inorganic Chemistry Frontiers, Vol. 6, Issue 12
  • DOI: 10.1039/c9qi00484j

Carbon dioxide electroreduction to C2 products over copper-cuprous oxide derived from electrosynthesized copper complex
journal, August 2019


Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products
journal, March 2019


Enhancing electroreduction of CO 2 over Bi 2 WO 6 nanosheets by oxygen vacancies
journal, January 2019

  • Chu, Mengen; Chen, Chunjun; Guo, Weiwei
  • Green Chemistry, Vol. 21, Issue 10
  • DOI: 10.1039/c9gc00479c

Alloy Nanocatalysts for the Electrochemical Oxygen Reduction (ORR) and the Direct Electrochemical Carbon Dioxide Reduction Reaction (CO 2 RR)
journal, December 2018

  • Kim, Cheonghee; Dionigi, Fabio; Beermann, Vera
  • Advanced Materials, Vol. 31, Issue 31
  • DOI: 10.1002/adma.201805617

Carbon dioxide splitting using an electro-thermochemical hybrid looping strategy
journal, January 2018

  • Luc, Wesley; Jouny, Matthew; Rosen, Jonathan
  • Energy & Environmental Science, Vol. 11, Issue 10
  • DOI: 10.1039/c8ee00532j

Cooperative CO2-to-ethanol conversion via enriched intermediates at molecule–metal catalyst interfaces
journal, December 2019


Emerging nanostructured carbon-based non-precious metal electrocatalysts for selective electrochemical CO 2 reduction to CO
journal, January 2019

  • Wang, Xinyue; Zhao, Qidong; Yang, Bin
  • Journal of Materials Chemistry A, Vol. 7, Issue 44
  • DOI: 10.1039/c9ta09681g

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

Strain engineering of metal-based nanomaterials for energy electrocatalysis
journal, January 2019

  • Xia, Zhonghong; Guo, Shaojun
  • Chemical Society Reviews, Vol. 48, Issue 12
  • DOI: 10.1039/c8cs00846a

Regulating C–C coupling in thermocatalytic and electrocatalytic CO x conversion based on surface science
journal, January 2019

  • Jiang, Yawen; Long, Ran; Xiong, Yujie
  • Chemical Science, Vol. 10, Issue 31
  • DOI: 10.1039/c9sc02014d

Promises of Main Group Metal–Based Nanostructured Materials for Electrochemical CO 2 Reduction to Formate
journal, November 2019


Microfabricated electrodes unravel the role of interfaces in multicomponent copper-based CO2 reduction catalysts
text, January 2018


Low-Coordinated Edge Sites on Ultrathin Palladium Nanosheets Boost Carbon Dioxide Electroreduction Performance
journal, July 2018

  • Zhu, Wenjin; Zhang, Lei; Yang, Piaoping
  • Angewandte Chemie International Edition, Vol. 57, Issue 36
  • DOI: 10.1002/anie.201806432