Synergistic Effects of Phase Transition and Electron-Spin Regulation on the Electrocatalysis Performance of Ternary Nitride

被引:45
作者
Ban, Jinjin [1 ,2 ]
Xu, Hongjie [1 ]
Cao, Guoqin [1 ]
Fan, Yameng [3 ,4 ]
Pang, Wei Kong [3 ]
Shao, Guosheng [1 ]
Hu, Junhua [1 ,2 ]
机构
[1] Zhengzhou Univ, State Ctr Int Cooperat Designer Low Carbon & Envir, Sch Mat Sci & Engn, Zhengzhou 450001, Peoples R China
[2] Longzihu New Energy Lab, Zhengzhou 450001, Peoples R China
[3] Univ Wollongong, Inst Superconducting & Elect Mat, Wollongong, NSW 2500, Australia
[4] Univ Surrey, Dept Chem & Proc Engn, Guildford GU2 7XH, England
基金
中国国家自然科学基金;
关键词
electrocatalysis; electron-spin regulation; phase transition; transition metal nitrides; OXYGEN REDUCTION; METAL NITRIDES; STATE; FRAMEWORKS; MN;
D O I
10.1002/adfm.202300623
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Transition metal nitrides (TMNs) have great potential use in energy storage and conversion owing to tunable electronic and bonding characteristics. Novel iron rich nitrides nanoparticles anchored on the N-doped porous carbon, named as (CoxFe1-x)(3)N@NPC (0 <= x < 0.5) are designed here. The synergistic effects of phase transition and electron-spin regulation on oxygen electrocatalysis are testified. A core-shell structure of (CoxFe1-x)(3)N with high dispersibility is induced by an intermediate phase transition process, which significantly suppresses coarsening of the metallic nitrides. The Co incorporation regulates d-band electrons spin polarization. The t(2g)(5)e(g)(1) of Fe-II with the ideal e(g) electron filling boosts intrinsic activity. (Co0.17Fe0.83)(3)N@NPC with optimal cobalt content holds electronic configuration with moderate e(g) electron filling (t(2g)(5)e(g)(1)), which balances the adsorption of *O-2 and the hydrogenation of *OH, improving bifunctional catalytic performances. Both liquid and solid-state zinc-air batteries assembled based (Co0.17Fe0.83)(3)N@NPC cathodes substantially deliver higher peak power density and remarkable energy density.
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页数:11
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