3D N-doped ordered mesoporous carbon supported single-atom Fe-N-C catalysts with superior performance for oxygen reduction reaction and zinc-air battery

被引:440
作者
Han, Junxing [1 ,2 ]
Bao, Hongliang [3 ]
Wang, Jian-Qiang [3 ]
Zheng, Lirong [4 ]
Sun, Shaorui [5 ]
Wang, Zhong Lin [1 ,2 ,6 ]
Sun, Chunwen [1 ,2 ]
机构
[1] Chinese Acad Sci, CAS Ctr Excellence Nanosci, Beijing Inst Nanoenergy & Nanosyst, Beijing 100083, Peoples R China
[2] Univ Chinese Acad Sci, Sch Nanosci & Technol, Beijing 100049, Peoples R China
[3] Chinese Acad Sci, Shanghai Inst Appl Phys, Key Lab Interfacial Phys & Technol, Shanghai 201800, Peoples R China
[4] Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China
[5] Beijing Univ Technol, Coll Environm & Energy Engn, Beijing Key Lab Green Catalysis & Separat, Beijing 100124, Peoples R China
[6] Georgia Inst Technol, Sch Mat Sci & Engn, Atlanta, GA 30332 USA
基金
美国国家科学基金会;
关键词
accessible active site; ordered mesoporous carbon; oxygen reduction reaction; single-atom electrocatalyst; zinc-air battery; EFFICIENT ELECTROCATALYST; ACTIVE-SITES; IRON; ARRAYS;
D O I
10.1016/j.apcatb.2020.119411
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Single-atom Fe-N-C electrocatalysts have emerged as the most promising oxygen reduction reaction (ORR) catalyst. However, the low Fe loading and inaccessibility of Fe-N-C sites limit the overall ORR activity. Here, we report an efficient single-atom electrocatalyst (Fe-N-C/N-OMC) with Fe-N-C sites embedded in three-dimensional (3D) N-doped ordered mesoporous carbon framework. Fe-N-C/N-OMC shows high half-wave potential, kinetic current density, turnover frequency and mass activity towards ORR in alkaline electrolyte. Experiments and theoretical calculations suggest that the ultra-high ORR activity stems from the boosted intrinsic activity of FeN4 sites by graphitic N dopants, high density of accessible active site generated by high Fe and N loadings and ordered mesoporous carbon structure as well as facilitated mass and electron transport in 3D interconnected pores. Fe-N-C/N-OMC also shows comparable ORR activity to PVC in acidic electrolyte. As the cathode for zinc-air battery, Fe-N-C/N-OMC exhibits high open-circuit voltage, high power density and remarkable durability.
引用
收藏
页数:10
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