pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper

Research output: Contribution to journalJournal article – Annual report year: 2019Researchpeer-review

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  • Author: Liu, Xinyan

    Stanford University, United States

  • Author: Schlexer, Philomena

    Stanford University, United States

  • Author: Xiao, Jianping

    Stanford University, United States

  • Author: Ji, Yongfei

    Stanford University, United States

  • Author: Wang, Lei

    Stanford University, United States

  • Author: Sandberg, Robert B.

    Stanford University, United States

  • Author: Tang, Michael T.

    Stanford University, United States

  • Author: Brown, Kristopher S.

    Stanford University, United States

  • Author: Peng, Hongjie

    Stanford University, United States

  • Author: Ringe, Stefan

    Stanford University, United States

  • Author: Hahn, Christopher

    SLAC National Accelerator Laboratory, United States

  • Author: Jaramillo, Thomas F.

    Stanford University, United States

  • Author: Nørskov, Jens K.

    Department of Physics, Technical University of Denmark, Fysikvej, 2800, Kgs. Lyngby, Denmark

  • Author: Chan, Karen

    Department of Physics, Technical University of Denmark, Fysikvej, 2800, Kgs. Lyngby, Denmark

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We present a microkinetic model for CO(2) reduction (CO(2)R) on Cu(211) towards C2 products, based on energetics estimated from an explicit solvent model. We show that the differences in both Tafel slopes and pH dependence for C1 vs C2 activity arise from differences in their multi-step mechanisms. We find the depletion in C2 products observed at high overpotential and high pH to arise from the 2nd order dependence of C-C coupling on CO coverage, which decreases due to competition from the C1 pathway. We further demonstrate that CO(2) reduction at a fixed pH yield similar activities, due to the facile kinetics for CO2 reduction to CO on Cu, which suggests C2 products to be favored for CO2R under alkaline conditions. The mechanistic insights of this work elucidate how reaction conditions can lead to significant enhancements in selectivity and activity towards higher value C2 products.
Original languageEnglish
Article number32
JournalNature Communications
Volume10
Issue number1
Number of pages9
ISSN2041-1723
DOIs
Publication statusPublished - 2019
CitationsWeb of Science® Times Cited: No match on DOI

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