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Title: Nature of the Active Sites for CO Reduction on Copper Nanoparticles; Suggestions for Optimizing Performance

Recent experiments show that the grain boundaries (GBs) of copper nanoparticles (NPs) lead to an outstanding performance in reducing CO 2 and CO to alcohol products. We report here multiscale simulations that simulate experimental synthesis conditions to predict the structure of a 10 nm Cu NP (158 555 atoms). To identify active sites, we first predict the CO binding at a large number of sites and select four exhibiting CO binding stronger than the (211) step surface. Then, we predict the formation energy of the *OCCOH intermediate as a descriptor for C–C coupling, identifying two active sites, both of which have an under-coordinated surface square site adjacent to a subsurface stacking fault. As a result, we then propose a periodic Cu surface (4 by 4 supercell) with a similar site that substantially decreases the formation energy of *OCCOH, by 0.14 eV.
Authors:
ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1]
  1. California Inst. of Technology (CalTech), Pasadena, CA (United States)
Publication Date:
Grant/Contract Number:
SC0004993
Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 34; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Research Org:
California Inst. of Technology (CalTech), Pasadena, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1467599

Cheng, Tao, Xiao, Hai, and Goddard, William A. Nature of the Active Sites for CO Reduction on Copper Nanoparticles; Suggestions for Optimizing Performance. United States: N. p., Web. doi:10.1021/jacs.7b03300.
Cheng, Tao, Xiao, Hai, & Goddard, William A. Nature of the Active Sites for CO Reduction on Copper Nanoparticles; Suggestions for Optimizing Performance. United States. doi:10.1021/jacs.7b03300.
Cheng, Tao, Xiao, Hai, and Goddard, William A. 2017. "Nature of the Active Sites for CO Reduction on Copper Nanoparticles; Suggestions for Optimizing Performance". United States. doi:10.1021/jacs.7b03300. https://www.osti.gov/servlets/purl/1467599.
@article{osti_1467599,
title = {Nature of the Active Sites for CO Reduction on Copper Nanoparticles; Suggestions for Optimizing Performance},
author = {Cheng, Tao and Xiao, Hai and Goddard, William A.},
abstractNote = {Recent experiments show that the grain boundaries (GBs) of copper nanoparticles (NPs) lead to an outstanding performance in reducing CO2 and CO to alcohol products. We report here multiscale simulations that simulate experimental synthesis conditions to predict the structure of a 10 nm Cu NP (158 555 atoms). To identify active sites, we first predict the CO binding at a large number of sites and select four exhibiting CO binding stronger than the (211) step surface. Then, we predict the formation energy of the *OCCOH intermediate as a descriptor for C–C coupling, identifying two active sites, both of which have an under-coordinated surface square site adjacent to a subsurface stacking fault. As a result, we then propose a periodic Cu surface (4 by 4 supercell) with a similar site that substantially decreases the formation energy of *OCCOH, by 0.14 eV.},
doi = {10.1021/jacs.7b03300},
journal = {Journal of the American Chemical Society},
number = 34,
volume = 139,
place = {United States},
year = {2017},
month = {8}
}