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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