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.

引用

页数：8

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