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Title: Electrochemical CO 2 reduction on Au surfaces: mechanistic aspects regarding the formation of major and minor products

In the future, industrial CO 2 electroreduction using renewable energy sources could be a sustainable means to convert CO 2 and water into commodity chemicals at room temperature and atmospheric pressure. This study focuses on the electrocatalytic reduction of CO 2 on polycrystalline Au surfaces, which have high activity and selectivity for CO evolution. Here, we explore the catalytic behavior of polycrystalline Au surfaces by coupling potentiostatic CO 2 electrolysis experiments in an aqueous bicarbonate solution with high sensitivity product detection methods. We observed the production of methanol, in addition to detecting the known products of CO 2 electroreduction on Au: CO, H 2 and formate. We suggest a mechanism that explains Au's evolution of methanol. Specifically, the Au surface does not favor C-O scission, and thus is more selective towards methanol than methane. These insights could aid in the design of electrocatalysts that are selective for CO 2 electroreduction to oxygenates over hydrocarbons.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [2] ; ORCiD logo [2]
  1. Stanford Univ., CA (United States). Dept. of Chemical Engineering
  2. Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis, Dept. of Chemical Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Grant/Contract Number:
AC02-76SF00515; 1066515; FA9550-10-1-0572
Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 19; Journal Issue: 24; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE; National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1369311

Cave, Etosha R., Montoya, Joseph H., Kuhl, Kendra P., Abram, David N., Hatsukade, Toru, Shi, Chuan, Hahn, Christopher, Nørskov, Jens K., and Jaramillo, Thomas F.. Electrochemical CO2 reduction on Au surfaces: mechanistic aspects regarding the formation of major and minor products. United States: N. p., Web. doi:10.1039/c7cp02855e.
Cave, Etosha R., Montoya, Joseph H., Kuhl, Kendra P., Abram, David N., Hatsukade, Toru, Shi, Chuan, Hahn, Christopher, Nørskov, Jens K., & Jaramillo, Thomas F.. Electrochemical CO2 reduction on Au surfaces: mechanistic aspects regarding the formation of major and minor products. United States. doi:10.1039/c7cp02855e.
Cave, Etosha R., Montoya, Joseph H., Kuhl, Kendra P., Abram, David N., Hatsukade, Toru, Shi, Chuan, Hahn, Christopher, Nørskov, Jens K., and Jaramillo, Thomas F.. 2017. "Electrochemical CO2 reduction on Au surfaces: mechanistic aspects regarding the formation of major and minor products". United States. doi:10.1039/c7cp02855e. https://www.osti.gov/servlets/purl/1369311.
@article{osti_1369311,
title = {Electrochemical CO2 reduction on Au surfaces: mechanistic aspects regarding the formation of major and minor products},
author = {Cave, Etosha R. and Montoya, Joseph H. and Kuhl, Kendra P. and Abram, David N. and Hatsukade, Toru and Shi, Chuan and Hahn, Christopher and Nørskov, Jens K. and Jaramillo, Thomas F.},
abstractNote = {In the future, industrial CO2 electroreduction using renewable energy sources could be a sustainable means to convert CO2 and water into commodity chemicals at room temperature and atmospheric pressure. This study focuses on the electrocatalytic reduction of CO2 on polycrystalline Au surfaces, which have high activity and selectivity for CO evolution. Here, we explore the catalytic behavior of polycrystalline Au surfaces by coupling potentiostatic CO2 electrolysis experiments in an aqueous bicarbonate solution with high sensitivity product detection methods. We observed the production of methanol, in addition to detecting the known products of CO2 electroreduction on Au: CO, H2 and formate. We suggest a mechanism that explains Au's evolution of methanol. Specifically, the Au surface does not favor C-O scission, and thus is more selective towards methanol than methane. These insights could aid in the design of electrocatalysts that are selective for CO2 electroreduction to oxygenates over hydrocarbons.},
doi = {10.1039/c7cp02855e},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 24,
volume = 19,
place = {United States},
year = {2017},
month = {1}
}

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