Welcome to the new version of CaltechAUTHORS. Login is currently restricted to library staff. If you notice any issues, please email coda@library.caltech.edu
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


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 (1.1 MB)
Name Size Download all
524.9 kB Download
590.3 kB Preview Download

Additional details

August 19, 2023
October 26, 2023