Highly ethylene‐selective electrocatalytic CO2 reduction enabled by isolated Cu‐S motifs in metal‐organic framework‐based precatalysts

Chun Fang Wen, Min Zhou, Peng Fei Liu, Yuanwei Liu, Xuefeng Wu, Fangxin Mao, Sheng Dai, Beibei Xu, Xue Lu Wang, Zheng Jiang, Peijun Hu, Shuang Yang, Hai Feng Wang, Huagui Yang

Research output: Contribution to journalArticlepeer-review

Abstract

Copper-based material is an efficient electrocatalyst for CO2 conversion to C2+ products, most of which will reconstruct to in-situ regenerate active species. It is a challenge to precisely design precatalyst to obtain active sites for CO2 reduction reaction (CO2RR). Herein, we develop a local sulfur doping strategy over the Cu-based metal-organic frameworks precatalyst that disperses stable Cu-S motif in the framework of HKUST-1 (S-HKUST-1). The precatalyst exhibits a high ethylene selectivity in H-type cell with maximum faradaic efficiency (FE) of 60.0%, and delivers a current density of 400 mA cm-2 with ethylene FE to 57.2% in a flow cell. Operando X-ray absorption results demonstrate that Cuδ+ species stabilized by Cu-S motif exist in S-HKUST-1 during CO2RR. Density functional theory calculations indicate the partially oxidized Cuδ+ at Cu/CuxSy interface is favorable for *CO intermediate coupling due to the modest distance of coupling sites and optimized adsorption energy.
Original languageEnglish
Article numbere202111700
JournalAngewandte Chemie International Edition
Volume61
Issue number2
Early online date23 Oct 2021
DOIs
Publication statusPublished - 10 Jan 2022

Keywords

  • General Chemistry
  • Catalysis

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