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

Cheng, Tao and Huang, Yufeng and Xiao, Hai and Goddard III, William A. (2017) Predicted Structures of the Active Sites Responsible for the Improved Reduction of Carbon Dioxide by Gold Nanoparticles. Journal of Physical Chemistry Letters, 8 (14). pp. 3317-3320. ISSN 1948-7185. https://resolver.caltech.edu/CaltechAUTHORS:20170706-080647539

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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.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/acs.jpclett.7b01335DOIArticle
http://pubs.acs.org/doi/abs/10.1021/acs.jpclett.7b01335PublisherArticle
http://pubs.acs.org/doi/suppl/10.1021/acs.jpclett.7b01335PublisherSupporting Information
ORCID:
AuthorORCID
Cheng, Tao0000-0003-4830-177X
Huang, Yufeng0000-0002-0373-2210
Xiao, Hai0000-0001-9399-1584
Goddard III, William A.0000-0003-0097-5716
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.
Group:JCAP
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
NSFACI-1053575
Issue or Number:14
Record Number:CaltechAUTHORS:20170706-080647539
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20170706-080647539
Official Citation:Predicted Structures of the Active Sites Responsible for the Improved Reduction of Carbon Dioxide by Gold Nanoparticles Tao Cheng, Yufeng Huang, Hai Xiao, and William A. Goddard, III The Journal of Physical Chemistry Letters 2017 8 (14), 3317-3320 DOI: 10.1021/acs.jpclett.7b01335
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:78791
Collection:CaltechAUTHORS
Deposited By: Donna Wrublewski
Deposited On:06 Jul 2017 16:38
Last Modified:03 Oct 2019 18:12

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