Fe2 Dimers for Non-Polar Diatomic O2 Electroreduction

被引：2
|
作者：
Fan, Ruxue [1 ]
Wang, Haiyan [3 ]
Zheng, Xiaozhong [1 ]
Chen, Jiadong [1 ]
Ou, Yang [4 ,5 ]
Wang, Yong [1 ,2 ]
Mao, Shanjun [1 ,2 ]
机构：
[1] Zhejiang Univ, Dept Chem, Inst Catalysis, Adv Mat & Catalysis Grp, Hangzhou 310028, Peoples R China
[2] Zhejiang Univ, Ctr Chem Frontier Technol, Hangzhou 310028, Peoples R China
[3] Zhejiang Normal Univ, Dept Chem, Key Lab, Minist Educ Adv Catalysis Mat, Jinhua 321004, Zhejiang, Peoples R China
[4] Zhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
[5] Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Hangzhou 310027, Peoples R China
来源：
CHEMSUSCHEM | 2022年 / 15卷 / 15期
基金：
中国国家自然科学基金; 国家重点研发计划;
关键词：
catalysis; electrochemistry; electroreduction; hydrogen atom transfer; oxygen reduction reaction; OXYGEN REDUCTION REACTION; TOTAL-ENERGY CALCULATIONS; CATALYSTS; ELECTROCATALYSIS; NANOCRYSTALS; REACTIVITY; TIO2;
D O I：
10.1002/cssc.202200532
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
Non-polar diatomic molecule activation is of great significance for catalysis. Despite the high atomic efficiency, the catalytic performance of single-atom catalysts is limited by insufficient receiving sites for diatomic molecule adsorption. Here, Fe-2 dimers were successfully synthesized through precisely regulating the metal loading on metal-organic frameworks. The unique role of metal dimers in activating diatomic O-2 molecules was explored. In alkaline electrolytes, the specific oxygen reduction reaction activity of Fe-2 dimers was 7 times higher than that of Fe-1 counterparts. The hydrogen atom transfer probes indicated a different activation mode for O-2 on Fe-1 and Fe-2 dimers, respectively. Theoretical calculation results revealed that Fe-2 dimers opened up a new reaction pathway by promoting the direct breaking of O=O bonds, thus avoiding the usual formation of *OOH intermediates, which helped explain the lower H2O2 yield and higher specific activity.
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页数：8
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