Achieving efficient alkaline hydrogen evolution reaction on long-range Ni sites in Ru clusters-immobilized Ni3N array catalyst

被引:22
作者
Gao, Xiaorui [1 ]
Zang, Wenjie [2 ]
Li, Xin [3 ]
Wang, Zhanke [4 ]
Zheng, Lirong [5 ]
Kou, Zongkui [6 ]
机构
[1] Changshu Inst Technol, Sch Elect & Informat Engn, Changshu 215500, Peoples R China
[2] Univ Calif Irvine, Dept Mat Sci & Engn, Irvine, CA 92697 USA
[3] Nanyang Technol Univ, Sch Phys & Math Sci, Singapore 637371, Singapore
[4] Wuhan Univ Technol, Sch Chem, Chem Engn & Life Sci, Wuhan 430070, Hubei, Peoples R China
[5] Chinese Acad Sci, Beijing Synchrotron Radiat Facil, Inst High Energy Phys, Beijing 100049, Peoples R China
[6] Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China
基金
中国国家自然科学基金;
关键词
Water adsorption; Hydrogen binding; Hydrogen evolution reaction; Water splitting; Electrocatalyst; NITRIDE; REDUCTION;
D O I
10.1016/j.cej.2022.138698
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Hydrogen (H-2) production from alkaline water electrocatalysis is economically appealing yet significantly hindered by the sluggish H2O adsorption and H* binding kinetics on active sites during hydrogen evolution reaction (HER). Herein, we interfacially immobilize Ru clusters on the hierarchical nickel nitride (Ru-Ni3N) nanosheet arrays via the filling of Ru3+ species into the metal vacancies of nickel hydroxide precursors and the subsequent controllable nitridation. The optimized Ru-Ni3N shows the outstanding HER performance, affording a 30-fold rise in the intrinsic activity of Ni sites, a outperforming-Pt/C overpotential at >= 125 mA cm(-2) while remaining a robust stability. We further establish by a combined study of density functional theory (DFT) calculations with experimental analyses that long-range Ni sites around Ru sites act as active sites via the electron delocalization, remarkably weakening the H2O adsorption and H* binding barriers for enhancing the alkaline HER kinetics. Moreover, it also demonstrates an excellent pH-universal HER and overall water splitting performance.
引用
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页数:8
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