期刊
CCS CHEMISTRY
卷 3, 期 12, 页码 199-207出版社
CHINESE CHEMICAL SOC
DOI: 10.31635/ccschem.020.202000589
关键词
copper sulfide; hollow structure; CO2 reduction; electrocatalysis; formate
资金
- National Natural Science Foundation of China [22002168, 21975259, 21673241]
- Innovation Academy for Green Manufacture of the Chinese Academy of Sciences [IAGM2020C17]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB20000000]
An hierarchical CuS hollow polyhedron was reported for electrocatalytic CO2 reduction in neutral pH aqueous media, showing high formate production efficiency. Experimental and theoretical analysis indicated that sulfur-doped Cu(111) facet played a key role in promoting formate selectivity.
Electroreduction of CO2 to target products with high activity and selectivity has techno-economic importance for renewable energy storage and CO2 utilization. Herein, we report a hierarchical CuS hollow polyhedron (CuS-HP) for electrocatalytic CO2 reduction (E-CO2R) in neutral pH aqueous media. Under E-CO2R conditions, CuS-HP undergoes structural reconstruction into sulfur-doped metallic Cu catalyst, which promotes formate production with Faradaic efficiency >90% in a wide potential range. The durability of the in situ evolved catalyst has been demonstrated by stable operation for 36 h at a formate partial current density of similar to 16 mA cm(-2) at -0.6 V versus reversible hydrogen electrode. Theoretical thermodynamic analysis reveals that the sulfur-doped Cu(111) facet is responsible for high formate selectivity by promoting formate production and suppressing hydrogen evolution.
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