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Title: Predicted Structures of the Active Sites Responsible for the Improved Reduction of Carbon Dioxide by Gold Nanoparticles

Gold (Au) nanoparticles (NPs) are known experimentally to reduce carbon dioxide (CO 2) to carbon monoxide (CO), with far superior performance to Au foils. To obtain guidance in designing improved CO 2 catalysts, we want to understand the nature of the active sites on Au NPs. Here, we employed multiscale atomistic simulations to computationally synthesize and characterize a 10 nm thick Au NP on a carbon nanotube (CNT) support, and then we located active sites from quantum mechanics (QM) calculations on 269 randomly selected sites. The standard scaling relation is that the formation energy of *COOH (ΔE*COOH) is proportional to the binding energy of *CO (Ebinding*CO); therefore, decreasing ΔE*COOH to boost the CO 2 reduction reaction (CO 2RR) causes an increase of Ebinding*CO that retards CO 2RR. We show that the NPs have superior CO 2RR because there are many sites at the twin boundaries that significantly break this scaling relation.
Authors:
ORCiD logo [1] ;  [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 Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 8; Journal Issue: 14; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
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:
1467601