Double layer charging driven carbon dioxide adsorption limits the rate of electrochemical carbon dioxide reduction on Gold

Ringe, Stefan; Morales-Guio, Carlos G.; Chen, Leanne D.; Fields, Meredith; Jaramillo, Thomas F.; Hahn, Christopher; Chan, Karen

doi:10.1038/s41467-019-13777-z

Double layer charging driven carbon dioxide adsorption limits the rate of electrochemical carbon dioxide reduction on Gold

Journal Article · Tue Jan 07 00:00:00 EST 2020 · Nature Communications

DOI:https://doi.org/10.1038/s41467-019-13777-z· OSTI ID:1575240

Ringe, Stefan ^[1]; Morales-Guio, Carlos G. ^[2]; Chen, Leanne D. ^[3]; Fields, Meredith ^[1]; Jaramillo, Thomas F. ^[1]; Hahn, Christopher ^[1]; Chan, Karen ^[4]

Stanford Univ., Stanford, CA (United States). SUNCAT Center for Interface Science and Catalysis, Dept. of Chemical Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis
Stanford Univ., Stanford, CA (United States). SUNCAT Center for Interface Science and Catalysis, Dept. of Chemical Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis; Univ. of California, Los Angeles, CA (United States). Dept. of Chemical and Biomolecular Engineering
California Inst. of Technology (CalTech), Pasadena, CA (United States). Div. of Chemistry and Chemical Engineering
Technical Univ. of Denmark, Lyngby (Denmark). CatTheory Center, Dept. of Physics

Electrochemical CO₂ reduction is a potential route to the sustainable production of valuable fuels and chemicals. Here, we perform CO₂ reduction experiments on Gold at neutral to acidic pH values to elucidate the long-standing controversy surrounding the rate-limiting step. We find the CO production rate to be invariant with pH on a Standard Hydrogen Electrode scale and conclude that it is limited by the CO₂ adsorption step. We present a new multi-scale modeling scheme that integrates ab initio reaction kinetics with mass transport simulations, explicitly considering the charged electric double layer. The model reproduces the experimental CO polarization curve and reveals the rate-limiting step to be *COOH to *CO at low overpotentials, CO₂ adsorption at intermediate ones, and CO₂ mass transport at high overpotentials. Finally, we show the Tafel slope to arise from the electrostatic interaction between the dipole of *CO₂ and the interfacial field. This work highlights the importance of surface charging for electrochemical kinetics and mass transport.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: Swiss National Science Foundation; USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515; SC0004993

OSTI ID:: 1575240

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 11; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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