期刊
ACS CATALYSIS
卷 9, 期 4, 页码 3744-3752出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b00407
关键词
hydrogen evolution reaction; reaction kinetics; pH-universal; DFT; transition metal phosphide
资金
- National Natural Science Foundation of China [21571145, 21633008]
- Large-scale Instrument and Equipment Sharing Foundation of Wuhan University
The development of precious-metal-free electrocatalysts with high-efficiency for hydrogen evolution reaction (HER) at all pHs is of great interest for the development of electrochemical overall splitting technologies. Despite that intense efforts have been made to developing cost-effective electrocatalysts toward HER under both acidic and alkaline electrolytes with high efficiency, electrocatalysts with remarkable performance in neutral media are rare. Herein, N atoms doped Co2P nanorod arrays grown on carbon cloth (N-Co2P/CC) have been successfully synthesized and further used as efficient electrocatalysts for HER at all pH values. Specially, the N-Co2P/CC exhibits an overpotential of 42 mV at the current density of 10 mA cm(-2) with long-term stability in 1.0 M PBS (phosphate-buffered solution), which is comparable to the benchmark Pt/CC. Density functional theory (DFT) calculations suggest nitrogen doping could tailor the electronic structure of Co2P, leading to optimized adsorption free energies of water (Delta G(*H2)(O)) and hydrogen (Delta G(*H)), facilitating hydrogen generation through the Volmer-Heyrovsky mechanism.
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