Cu metal embedded in oxidized matrix catalyst to promote CO2 activation and CO dimerization for electrochemical reduction of CO2

Xiao, Hai; Goddard, William A.; Cheng, Tao; Liu, Yuanyue

doi:10.1073/pnas.1702405114

Title: Cu metal embedded in oxidized matrix catalyst to promote CO₂ activation and CO dimerization for electrochemical reduction of CO₂

Journal Article · Mon Jun 12 00:00:00 EDT 2017 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1702405114· OSTI ID:1465782

^[1];

^[1]; Liu, Yuanyue ^[1]

California Inst. of Technology (CalTech), Pasadena, CA (United States)

We propose and validate with quantum mechanics methods a unique catalyst for electrochemical reduction of CO₂ (CO₂RR) in which selectivity and activity of CO and C₂ products are both enhanced at the borders of oxidized and metallic surface regions. This Cu metal embedded in oxidized matrix (MEOM) catalyst is consistent with observations that Cu₂O-based electrodes improve performance. However, we show that a fully oxidized matrix (FOM) model would not explain the experimentally observed performance boost, and we show that the FOM is not stable under CO2 reduction conditions. This electrostatic tension between the Cu⁺ and Cu0 surface sites responsible for the MEOM mechanism suggests a unique strategy for designing more efficient and selective electrocatalysts for CO₂RR to valuable chemicals (HCO_x), a critical need for practical environmental and energy applications.

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Research Organization:: California Institute of Technology (CalTech), Pasadena, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: SC0004993

OSTI ID:: 1465782

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Vol. 114, Issue 26; ISSN 0027-8424

Publisher:: National Academy of Sciences, Washington, DC (United States)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 280 works

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Title: Cu metal embedded in oxidized matrix catalyst to promote CO₂ activation and CO dimerization for electrochemical reduction of CO₂