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Title: Understanding trends in electrochemical carbon dioxide reduction rates

Electrochemical carbon dioxide reduction to fuels presents one of the great challenges in chemistry. Herein we present an understanding of trends in electrocatalytic activity for carbon dioxide reduction over different metal catalysts that rationalize a number of experimental observations including the selectivity with respect to the competing hydrogen evolution reaction. We also identify two design criteria for more active catalysts. The understanding is based on density functional theory calculations of activation energies for electrochemical carbon monoxide reduction as a basis for an electrochemical kinetic model of the process. Furthermore, we develop scaling relations relating transition state energies to the carbon monoxide adsorption energy and determine the optimal value of this descriptor to be very close to that of copper.
Authors:
 [1] ;  [1] ;  [2] ;  [3] ; ORCiD logo [4] ;  [1]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
  2. Stanford Univ., Stanford, CA (United States); Tsinghua Univ., Beijing (China)
  3. Stanford Univ., Stanford, CA (United States); Zhejiang Univ., Hangzhou (China)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Grant/Contract Number:
AC02-76SF00515
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; electrocatalysis; electrochemistry
OSTI Identifier:
1368688

Liu, Xinyan, Xiao, Jianping, Peng, Hongjie, Hong, Xin, Chan, Karen, and Norskov, Jens K. Understanding trends in electrochemical carbon dioxide reduction rates. United States: N. p., Web. doi:10.1038/ncomms15438.
Liu, Xinyan, Xiao, Jianping, Peng, Hongjie, Hong, Xin, Chan, Karen, & Norskov, Jens K. Understanding trends in electrochemical carbon dioxide reduction rates. United States. doi:10.1038/ncomms15438.
Liu, Xinyan, Xiao, Jianping, Peng, Hongjie, Hong, Xin, Chan, Karen, and Norskov, Jens K. 2017. "Understanding trends in electrochemical carbon dioxide reduction rates". United States. doi:10.1038/ncomms15438. https://www.osti.gov/servlets/purl/1368688.
@article{osti_1368688,
title = {Understanding trends in electrochemical carbon dioxide reduction rates},
author = {Liu, Xinyan and Xiao, Jianping and Peng, Hongjie and Hong, Xin and Chan, Karen and Norskov, Jens K.},
abstractNote = {Electrochemical carbon dioxide reduction to fuels presents one of the great challenges in chemistry. Herein we present an understanding of trends in electrocatalytic activity for carbon dioxide reduction over different metal catalysts that rationalize a number of experimental observations including the selectivity with respect to the competing hydrogen evolution reaction. We also identify two design criteria for more active catalysts. The understanding is based on density functional theory calculations of activation energies for electrochemical carbon monoxide reduction as a basis for an electrochemical kinetic model of the process. Furthermore, we develop scaling relations relating transition state energies to the carbon monoxide adsorption energy and determine the optimal value of this descriptor to be very close to that of copper.},
doi = {10.1038/ncomms15438},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {2017},
month = {5}
}

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