期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 297, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120452
关键词
Nitrogen reduction reaction; Electrocatalyst; Oxygen vacancy; Prussian blue analogue; CoFe2O4
资金
- National Natural Science Foundation of China [21878063]
- Natural Science Foundation of Heilongjiang Province of China
- Taishan Scholars Pro-gram of Shandong Province [tsqn201909119]
- Key Program of Shandong Provincial Natural Science Foundation [ZR2020KB011]
The study demonstrates the excellent activity and stability of the hollow bimetallic CoFe2O4 nanocube in nitrogen reduction reaction, attributed to improved nitrogen adsorption and activation, unoccupied d orbitals of transition metal components, reformed electronic structure by oxygen vacancies, and electron injection facilitated by conductive carbon wrapper. Both experimental and theoretical investigations confirm the mechanism underlying the enhancement in catalytic activity, making the design strategy of C@CoFe2O4-x nanocube efficient and valid.
Electrocatalytic nitrogen reduction reaction is increasingly deemed as a promising route for massive ammonia synthesis. Herein, hollow bimetallic CoFe2O4 nanocube derived from prussian blue analogue is elaborately wrapped by thin carbon layer and modified by rich oxygen vacancies, achieving splendid ammonia yield rate of 30.97 mu g h-1 mgcat.- 1 and Faradaic efficiency of 11.65 % at -0.4 V versus reversible hydrogen electrode in 0.1 M Na2SO4. In addition, C@CoFe2O4-x nanocube can withstand long-term and repetitive electrolysis without obvious structure collapse, constituent change and activity decay. The prominent activity is strongly associated with improved nitrogen adsorption and activation, collaboratively benefiting from the intrinsic unoccupied d orbitals of transition metal components, reformative electronic structure by oxygen vacancies and elevated electron injection possibility into the antibonding orbital of nitrogen molecule via conductive carbon wrapper. Both actual experiments and theoretical investigations attest the catalytic activity improvement mechanism, rendering the C@CoFe2O4-x nanocube design strategy efficient and valid.
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