Multi-elemental Electronic Coupling for Enhanced Hydrogen Generation

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论文题目:Multi-elemental Electronic Coupling for Enhanced Hydrogen Generation

论文作者:Huan Li, Minghao Hu, Bo Cao, Peng Jing, Baocang Liu, Rui Gao, Jun Zhang, Xiaomeng Shi, Yaping Du*

发表期刊:Small, 17(11), 2006617, 2021    

Abstract: 

A robust polyaniline-assisted strategy is developed to construct a  self-supported electrode constituting a nitrogen, phosphorus, sulfur  tri-doped thin graphitic carbon layer encapsulated sulfur-doped  molybdenum phosphide nanosheet array (NPSCL@S-MoP NSs/CC) with  accessible nanopores, desirable chemical compositions, and stable  composite structure for efficient hydrogen evolution reaction (HER). The  multiple electronic coupling effects of S-MoP with N, P, S tri-dopants  afford effective regulation on their electrocatalytic performance by  endowing abundant accessible active sites, outstanding charge-transfer  property, and d-band center downshift with a thermodynamically favorable  hydrogen adsorption free energy (Delta G(H*)) for efficient hydrogen  evolution catalysis. As a result, the NPSCL@S-MoP NSs/CC electrode  exhibits overpotentials as low as 65, 114, and 49 mV at a geometric  current density of 10 mA cm(-2) and small Tafel slopes of 49.5, 69.3,  and 53.8 mV dec(-1) in 0.5 m H2SO4, 1.0 m PBS, and 1.0 m KOH,  respectively, which could maintain 50 h of stable performance, almost  outperforming all MoP-based catalysts reported so far. This study  provides a valuable methodology to produce interacted multi-heteroatomic  doped graphitic carbon-transition metal phosphide electrocatalysts with  superior HER performance in a wide pH range.

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