Activity and Selectivity Control in CO 2 Electroreduction to Multicarbon Products over CuO x Catalysts via Electrolyte Design

Gao, Dunfeng; McCrum, Ian T.; Deo, Shyam; Choi, Yong-Wook; Scholten, Fabian; Wan, Weiming; Chen, Jingguang G.; Janik, Michael J.; Roldan Cuenya, Beatriz

doi:10.1021/acscatal.8b02587

Title: Activity and Selectivity Control in CO ₂ Electroreduction to Multicarbon Products over CuO _x Catalysts via Electrolyte Design

Journal Article · Tue Sep 11 00:00:00 EDT 2018 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.8b02587· OSTI ID:1484885

^[1]; McCrum, Ian T. ^[2]; Deo, Shyam ^[3]; Choi, Yong-Wook ^[4]; Scholten, Fabian ^[4]; Wan, Weiming ^[5]; Chen, Jingguang G. ^[6]; Janik, Michael J. ^[3];

^[4]

Max Planck Society, Berlin (Germany). Fritz-Haber Inst., Dept. of Interface Science; Ruhr-Univ., Bochum (Germany). Dept. of Physics
Pennsylvania State Univ., University Park, PA (United States). Dept. of Chemical Engineering
ennsylvania State Univ., University Park, PA (United States). Dept. of Chemical Engineering
Max Planck Society, Berlin (Germany). Fritz-Haber Inst., Dept. of Interface Science; Ruhr-Univ., Bochum (Germany). Dept. of Physics
Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.

The CO₂ electroreduction reaction (CO₂RR) to chemicals and fuels is of both fundamental and practical significance, since it would lead to a more efficient storage of renewable energy while closing the carbon cycle. Here we report enhanced activity and selectivity for the CO₂RR to multicarbon hydrocarbons and alcohols (~69% Faradaic efficiency and -45.5 mA cm^–2 partial current density for C₂₊ at -1.0 V vs RHE) over O₂-plasma-activated Cu catalysts via electrolyte design. Increasing the size of the alkali-metal cations in the electrolyte, in combination with the presence of subsurface oxygen species which favor their adsorption, significantly improved C–C coupling on CuO_x electrodes. The coexistence of Cs⁺ and I^– induced drastic restructuring of the CuO_x surface, the formation of shaped particles containing stable CuI species, and a more favorable stabilization of the reaction intermediates and concomitant high C₂₊ selectivity. This work, combining both experiment and density functional theory, provides insights into the active sites and reaction mechanism of oxide-derived Cu catalysts for the CO₂RR.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

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

Grant/Contract Number:: SC0012704

OSTI ID:: 1484885

Report Number(s):: BNL-209655-2018-JAAM

Journal Information:: ACS Catalysis, Vol. 8, Issue 11; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 117 works

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Title: Activity and Selectivity Control in CO ₂ Electroreduction to Multicarbon Products over CuO _x Catalysts via Electrolyte Design