Published July 20, 2017 | Supplemental Material
Journal Article Open

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

  • 1. ROR icon California Institute of Technology
An error occurred while generating the citation.

Abstract

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 (E^(binding)_(*CO)); therefore, decreasing ΔE_(*COOH) to boost the CO_2 reduction reaction (CO_2RR) causes an increase of E^(binding)_(*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.

Additional Information

© 2017 American Chemical Society. Received: May 29, 2017; Accepted: July 4, 2017; Published: July 4, 2017. This work was supported by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award No. DE-SC0004993. This work used the Extreme Science and Engineering Discovery Environment (XSEDE) which is supported by National Science Foundation grant number ACI-1053575, and the Zwicky Astrophysics supercomputer at Caltech. The authors declare no competing financial interest.

Attached Files

Supplemental Material - jz-2017-013355-SI-FRO-wag.docx

Supplemental Material - jz7b01335_si_001.pdf

Files

jz7b01335_si_001.pdf
Files (1.1 MB)
Name Size Download all
md5:5387dc309b763e242db3af69b9214a2f
524.9 kB Download
md5:bdd81e24205f79045053451dc1c181e4
590.3 kB Preview Download

Additional details

Created:
August 19, 2023
Modified:
April 25, 2025