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Embedding Covalency into Metal Catalysts for Efficient Electrochemical Conversion of CO_2

Lim, Hyung-Kyu and Shin, Hyeyoung and Goddard, William A., III and Hwang, Yun Jeong and Min, Byoung Koun and Kim, Hyungjun (2014) Embedding Covalency into Metal Catalysts for Efficient Electrochemical Conversion of CO_2. Journal of the American Chemical Society, 136 (32). pp. 11355-11361. ISSN 0002-7863. https://resolver.caltech.edu/CaltechAUTHORS:20140911-134457686

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Abstract

CO_2 conversion is an essential technology to develop a sustainable carbon economy for the present and the future. Many studies have focused extensively on the electrochemical conversion of CO_2 into various useful chemicals. However, there is not yet a solution of sufficiently high enough efficiency and stability to demonstrate practical applicability. In this work, we use first-principles-based high-throughput screening to propose silver-based catalysts for efficient electrochemical reduction of CO_2 to CO while decreasing the overpotential by 0.4–0.5 V. We discovered the covalency-aided electrochemical reaction (CAER) mechanism in which p-block dopants have a major effect on the modulating reaction energetics by imposing partial covalency into the metal catalysts, thereby enhancing their catalytic activity well beyond modulations arising from d-block dopants. In particular, sulfur or arsenic doping can effectively minimize the overpotential with good structural and electrochemical stability. We expect this work to provide useful insights to guide the development of a feasible strategy to overcome the limitations of current technology for electrochemical CO_2 conversion.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/ja503782wDOIArticle
http://pubs.acs.org/doi/abs/10.1021/ja503782wPublisherArticle
http://pubs.acs.org/doi/suppl/10.1021/ja503782wPublisherSupporting Information
Alternate Title:Embedding Covalency into Metal Catalysts for Efficient Electrochemical Conversion of CO2
Additional Information:© 2014 American Chemical Society. Received: April 15, 2014; Published: July 25, 2014. This work was supported by the Global Frontier R&D Program (2013M3A6B1078884) on Center for Hybrid Interface Materials (HIM) funded by the Ministry of Science, ICT & Future Planning, and by the institutional program of the Korea Institute of Science and Technology (KIST). We also acknowledge the Supercomputing Center/Korea Institute of Science and Technology Information with supercomputing resources including technical support (KSC-2013-G3-002).
Funders:
Funding AgencyGrant Number
Ministry of Science2013M3A6B1078884
ICT & Future PlanningUNSPECIFIED
Korea Institute of Science and Technology (KIST)UNSPECIFIED
Supercomputing Center/Korea Institute of Science and Technology InformationKSC-2013-G3-002
Issue or Number:32
Record Number:CaltechAUTHORS:20140911-134457686
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20140911-134457686
Official Citation:Embedding Covalency into Metal Catalysts for Efficient Electrochemical Conversion of CO2 Hyung-Kyu Lim, Hyeyoung Shin, William A. Goddard, III, Yun Jeong Hwang, Byoung Koun Min, and Hyungjun Kim Journal of the American Chemical Society 2014 136 (32), 11355-11361
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:49615
Collection:CaltechAUTHORS
Deposited By: Jason Perez
Deposited On:11 Sep 2014 23:21
Last Modified:03 Oct 2019 07:15

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