Activity and Selectivity Control in CO2 Electroreduction to Multicarbon Products over CuOx Catalysts via Electrolyte Design

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

Research output: Contribution to journalArticlepeer-review

55 Scopus citations

Abstract

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 CuOx electrodes. The coexistence of Cs+ and I- induced drastic restructuring of the CuOx 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.

Original languageEnglish (US)
Pages (from-to)10012-10020
Number of pages9
JournalACS Catalysis
Volume8
Issue number11
DOIs
StatePublished - Nov 2 2018

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)

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