Mechanistic insights into electrochemical reduction of CO 2 over Ag using density functional theory and transport models

Singh, Meenesh R.; Goodpaster, Jason D.; Weber, Adam Z.; Head-Gordon, Martin; Bell, Alexis T.

doi:10.1073/pnas.1713164114

Title: Mechanistic insights into electrochemical reduction of CO ₂ over Ag using density functional theory and transport models

Journal Article · 01 October 2017 · Proceedings of the National Academy of Sciences of the United States of America

DOI: https://doi.org/10.1073/pnas.1713164114 · OSTI ID:1396063

^[1]; Goodpaster, Jason D. ^[2]; Weber, Adam Z. ^[3];

^[4];

^[5]

Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, Berkeley, CA 94720,, Department of Chemical Engineering, University of Illinois at Chicago, Chicago, IL 60607,
Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, Berkeley, CA 94720,, Department of Chemistry, University of Minnesota, Minneapolis, MN 55455,
Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, Berkeley, CA 94720,
Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, Berkeley, CA 94720,, Department of Chemistry, University of California, Berkeley, CA 94720,
Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, Berkeley, CA 94720,, Department of Chemical and Biomolecular Engineering, University of California, Berkeley, CA 94720

Significance Chemical storage of solar energy can be achieved by electrochemical reduction of CO ₂ to CO and H ₂ , and subsequent conversion of this mixture to fuels. Identifying optimal conditions for electrochemical cell operation requires knowledge of the CO ₂ reduction mechanism and the influence of all factors controlling cell performance. We report a multiscale model for predicting the current densities for H ₂ and CO formation from first principles. Our approach brings together a quantum-chemical analysis of the reaction pathway, a microkinetic model of the reaction dynamics, and a continuum model for mass transport of all species through the electrolyte. This model is essential for identifying a physically correct representation of product current densities dependence on the cell voltage and CO ₂ partial pressure.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231; SC0004993

OSTI ID:: 1396063

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 42 Vol. 114; ISSN 0027-8424

Publisher:: Proceedings of the National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Mechanistic insights into electrochemical reduction of CO 2 over Ag using density functional theory and transport models

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Title: Mechanistic insights into electrochemical reduction of CO ₂ over Ag using density functional theory and transport models