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Surface Ligand Promotion of Carbon Dioxide Reduction through Stabilizing Chemisorbed Reactive Intermediates

Wang, Zhijiang and Wu, Lina and Sun, Kun and Chen, Ting and Jiang, Zhaohua and Cheng, Tao and Goddard, William A., III (2018) Surface Ligand Promotion of Carbon Dioxide Reduction through Stabilizing Chemisorbed Reactive Intermediates. Journal of Physical Chemistry Letters, 9 (11). pp. 3057-3061. ISSN 1948-7185. https://resolver.caltech.edu/CaltechAUTHORS:20180522-100408414

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Abstract

We have explored functionalizing metal catalysts with surface ligands as an approach to facilitate electrochemical carbon dioxide reduction reaction (CO_2RR). To provide a molecular level understanding of the mechanism by which this enhancement occurs, we combine in situ spectroscopy analysis with an interpretation based on quantum mechanics (QM) calculations. We find that a surface ligand can play a critical role in stabilizing the chemisorbed CO_2, which facilitates CO_2 activation and leads to a 0.3 V decrease in the overpotential for carbon monoxide (CO) formation. Moreover, the presence of the surface ligand leads to nearly exclusive CO production. At −0.6 V (versus reversible hydrogen electrode, RHE), CO is the only significant product with a faradic efficiency of 93% and a current density of 1.9 mA cm^(–2). This improvement corresponds to 53-fold enhancement in turnover frequency compared with the Ag nanoparticles (NPs) without surface ligands.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acs.jpclett.8b00959DOIArticle
https://pubs.acs.org/doi/suppl/10.1021/acs.jpclett.8b00959PublisherSupporting Information
ORCID:
AuthorORCID
Wang, Zhijiang0000-0001-9314-7922
Chen, Ting0000-0002-9599-871X
Cheng, Tao0000-0003-4830-177X
Goddard, William A., III0000-0003-0097-5716
Additional Information:© 2018 American Chemical Society. Received: March 28, 2018; Accepted: May 22, 2018; Published: May 22, 2018. T.C. and W.A.G. were 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. Z.W. acknowledges financial support from the Open Project of State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology (No. HC201813). L.W. acknowledges financial support from the National Natural Science Foundation of China (No. 81771903) and Wuliande Foundation of Harbin Medical University (No. WLD-QN1404). The authors declare no competing financial interests.
Group:JCAP
Funders:
Funding AgencyGrant Number
Joint Center for Artificial Photosynthesis (JCAP)UNSPECIFIED
Department of Energy (DOE)DE-SC0004993
NSFACI-1053575
State Key Laboratory of Urban Water Resource and EnvironmentUNSPECIFIED
Harbin Institute of TechnologyHC201813
National Natural Science Foundation of China81771903
Wuliande Foundation of Harbin Medical UniversityWLD-QN1404
Other Numbering System:
Other Numbering System NameOther Numbering System ID
WAG1285
Issue or Number:11
Record Number:CaltechAUTHORS:20180522-100408414
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20180522-100408414
Official Citation:Surface Ligand Promotion of Carbon Dioxide Reduction through Stabilizing Chemisorbed Reactive Intermediates. Zhijiang Wang, Lina Wu, Kun Sun, Ting Chen, Zhaohua Jiang, Tao Cheng, and William A. Goddard, III. The Journal of Physical Chemistry Letters 2018 9 (11), 3057-3061. DOI: 10.1021/acs.jpclett.8b00959
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:86542
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:22 May 2018 17:14
Last Modified:09 Mar 2020 13:18

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