Boron-Induced Electronic-Structure Reformation of CoP Nanoparticles Drives Enhanced pH-Universal Hydrogen Evolution

被引:289
作者
Cao, Erping [1 ]
Chen, Zhimin [1 ]
Wu, Hao [1 ]
Yu, Peng [2 ]
Wang, Ying [1 ]
Xiao, Fei [1 ]
Chen, Shuo [1 ]
Du, Shichao [1 ]
Xie, Ying [1 ]
Wu, Yiqun [1 ]
Ren, Zhiyu [1 ]
机构
[1] Heilongjiang Univ, Sch Chem & Mat Sci, Minist Educ China, Key Lab Funct Inorgan Mat Chem, Harbin 150080, Peoples R China
[2] Harbin Normal Univ, Sch Phys & Elect Engn, Minist Educ China, Key Lab Photon & Elect Bandgap Mat, Harbin 150025, Peoples R China
基金
中国国家自然科学基金;
关键词
B-doping; carbon nanotubes (CNTs); electronic structure reformation; hydrogen evolution reaction (HER); transition-metal phosphide catalysts; N-DOPED CARBON; CATALYTIC-ACTIVITY; NANOWIRE ARRAYS; DESIGN; ELECTROCATALYSTS; PERFORMANCE; GRAPHENE; OXYGEN;
D O I
10.1002/anie.201915254
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Even though transition-metal phosphides (TMPs) have been developed as promising alternatives to Pt catalyst for the hydrogen evolution reaction (HER), further improvement of their performance requires fine regulation of the TMP sites related to their specific electronic structure. Herein, for the first time, boron (B)-modulated electrocatalytic characteristics in CoP anchored on the carbon nanotubes (B-CoP/CNT) with impressive HER activities over a wide pH range are reported. The HER performance surpasses commercial Pt/C in both neutral and alkaline media at large current density (>100 mA cm(-2)). A combined experimental and theoretical study identified that the B dopant could reform the local electronic configuration and atomic arrangement of bonded Co and adjacent P atoms, enhance the electrons' delocalization capacity of Co atoms for high electrical conductivity, and optimize the free energy of H adsorption and H-2 desorption on the active sites for better HER kinetics.
引用
收藏
页码:4154 / 4160
页数:7
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