Predicted Structures of the Active Sites Responsible for the Improved Reduction of Carbon Dioxide by Gold Nanoparticles
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
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Additional details
- Eprint ID
- 78791
- DOI
- 10.1021/acs.jpclett.7b01335
- Resolver ID
- CaltechAUTHORS:20170706-080647539
- Department of Energy (DOE)
- DE-SC0004993
- NSF
- ACI-1053575
- Created
-
2017-07-06Created from EPrint's datestamp field
- Updated
-
2021-11-15Created from EPrint's last_modified field
- Caltech groups
- JCAP