Metal-Organic Framework-Derived CuS Nanocages for Selective CO2 Electroreduction to Formate

被引：36
作者：
Zhang, Xing [1 ,2 ]
Sa, Rongjian [1 ,3 ]
Zhou, Feng [1 ,2 ]
Rui, Yuan [1 ]
Liu, Ruixia [4 ]
Wen, Zhenhai [1 ]
Wang, Ruihu [1 ,2 ,4 ]
机构：
[1] Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Minjiang Univ, Ocean Coll, Inst Oceanog, Fuzhou 350108, Fujian, Peoples R China
[4] Chinese Acad Sci, Innovat Acad Green Manufacture, Beijing 100190, Peoples R China
来源：
CCS CHEMISTRY | 2021年 / 3卷 / 12期
基金：
中国国家自然科学基金;
关键词：
copper sulfide; hollow structure; CO2; reduction; electrocatalysis; formate; CARBON-DIOXIDE; ELECTROCHEMICAL REDUCTION; ELECTROCATALYTIC CONVERSION; CATALYST; MONOXIDE; METHANOL; DESIGN;
D O I：
10.31635/ccschem.020.202000589
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
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.
引用
收藏
页码：199 / 207
页数：9
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