Efficient Electrocatalytic Reduction of CO2 to Ethane over Nitrogen-Doped Fe2O3

被引:67
|
作者
Chen, Peng [1 ,2 ]
Zhang, Pei [1 ]
Kang, Xinchen [1 ,2 ]
Zheng, Lirong [5 ]
Mo, Guang [5 ]
Wu, Ruizhi [1 ,2 ]
Tai, Jing [1 ]
Han, Buxing [1 ,2 ,3 ,4 ]
机构
[1] Chinese Acad Sci, Inst Chem, CAS Res Educ Ctr Excellence Mol Sci, Beijing Natl Lab Mol Sci,Key Lab Colloid Interface, Beijing 100190, Peoples R China
[2] Univ Chinese Acad Sci, Sch Chem, Beijing 100049, Peoples R China
[3] East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 200062, Peoples R China
[4] Inst Ecochongming, Shanghai 202162, Peoples R China
[5] Inst High Energy Phys, Chinese Acad Sci, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China
基金
中国国家自然科学基金;
关键词
OXYGEN REDUCTION; ELECTROCHEMICAL REDUCTION; CATALYTIC SITES; ELECTROREDUCTION; IRON; IDENTIFICATION; DENSITY;
D O I
10.1021/jacs.2c05373
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Non-copper electrocatalysts are seldom reported to generate C2+ products, and the efficiency over these catalysts is low. In this work, we report a nitrogen-doped gamma-Fe2O3 (xFe2O3-N@CN) electrocatalyst, which yield C2H6 as the major product in an H-cell. At -2.0 V vs Ag/Ag+, the Faradaic efficiency (FE) for ethane reaches 42% with a current density of 32 mA cm(-2). This is the first report about selective CO2 reduction to ethane (C2H6) over an iron-based catalyst. The results showed that the catalyst possessing FeO1.5-nNn sites enriched with oxygen vacancies was beneficial for the stabilization of *COOH intermediates. The exposure of two adjacent surfaces of Fe atoms was conducive to lowering the energy barrier for C-C coupling over FeO1.5-nNn sites, facilitating the generation of C2H6. This work provides a strategy for the design of a novel iron-based catalyst with tunable local coordination and electronic structures for converting CO2 into C-2 products in the CO2RR.
引用
收藏
页码:14769 / 14777
页数:9
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