CoP-Doped MOF-Based Electrocatalyst for pH-Universal Hydrogen Evolution Reaction

被引:640
作者
Liu, Teng [1 ,2 ]
Li, Peng [1 ]
Yao, Na [1 ]
Cheng, Gongzhen [1 ]
Chen, Shengli [1 ]
Luo, Wei [1 ,2 ]
Yin, Yadong [2 ]
机构
[1] Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Hubei, Peoples R China
[2] Univ Calif Riverside, Dept Chem, Riverside, CA 92521 USA
基金
中国国家自然科学基金;
关键词
DFT; hydrogen evolution reaction; metal-organic frameworks; pH-universal; transition metal phosphides; METAL-ORGANIC FRAMEWORKS; CATALYTIC-ACTIVITY; HIGHLY EFFICIENT; NANOWIRE ARRAY; CARBON; GRAPHENE; PERFORMANCE; OXIDATION; CATHODE; HYBRIDS;
D O I
10.1002/anie.201901409
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Although electrocatalysts based on transition metal phosphides (TMPs) with cationic/anionic doping have been widely studied for hydrogen evolution reaction (HER), the origin of performance enhancement still remains elusive mainly due to the random dispersion of dopants. Herein, we report a controllable partial phosphorization strategy to generate CoP species within the Co-based metal-organic framework (Co-MOF). Density functional theory calculations and experimental results reveal that the electron transfer from CoP to Co-MOF through N-P/N-Co bonds could lead to the optimized adsorption energy of H2O (Delta G(H2O*)) and hydrogen (Delta G(H*)), which, together with the unique porous structure of Co-MOF, contributes to the remarkable HER performance with an overpotential of 49 mV at a current density of 10 mA cm(-2) in 1 M phosphate buffer solution (PBS, pH 7.0). The excellent catalytic performance exceeds almost all the documented TMP-based and non-noble-metal-based electrocatalysts. In addition, the CoP/Co-MOF hybrid also displays Pt-like performance in 0.5 M H2SO4 and 1 M KOH, with the overpotentials of 27 and 34 mV, respectively, at a current density of 10 mA cm(-2).
引用
收藏
页码:4679 / 4684
页数:6
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