In:
Angewandte Chemie, Wiley, Vol. 134, No. 2 ( 2022-01-10)
Abstract:
Copper‐based materials are efficient electrocatalysts for the conversion of CO 2 to C 2+ products, and most these materials are reconstructed in situ to regenerate active species. It is a challenge to precisely design precatalysts to obtain active sites for the CO 2 reduction reaction (CO 2 RR). Herein, we develop a strategy based on local sulfur doping of a Cu‐based metal–organic framework precatalyst, in which the stable Cu−S motif is dispersed in the framework of HKUST‐1 (S‐HKUST‐1). The precatalyst exhibits a high ethylene selectivity in an H‐type cell with a maximum faradaic efficiency (FE) of 60.0 %, and delivers a current density of 400 mA cm −2 with an ethylene FE up to 57.2 % in a flow cell. Operando X‐ray absorption results demonstrate that Cu δ+ species stabilized by the Cu−S motif exist in S‐HKUST‐1 during CO 2 RR. Density functional theory calculations indicate the partially oxidized Cu δ+ at the Cu/Cu x S y interface is favorable for coupling of the *CO intermediate due to the modest distance between coupling sites and optimized adsorption energy.
Type of Medium:
Online Resource
ISSN:
0044-8249
,
1521-3757
DOI:
10.1002/ange.202111700
Language:
English
Publisher:
Wiley
Publication Date:
2022
detail.hit.zdb_id:
505868-5
detail.hit.zdb_id:
506609-8
detail.hit.zdb_id:
514305-6
detail.hit.zdb_id:
505872-7
detail.hit.zdb_id:
1479266-7
detail.hit.zdb_id:
505867-3
detail.hit.zdb_id:
506259-7
Permalink