It has been of interest in seeking electrocatalysts that could exercise equally high-efficient and durable hydrogen evolution upon nonselective electrolytes in both acidic and alkaline environments. Herein, we report ...It has been of interest in seeking electrocatalysts that could exercise equally high-efficient and durable hydrogen evolution upon nonselective electrolytes in both acidic and alkaline environments. Herein, we report a facile strategy to fabricate cobalt tungsten phosphides (CoxW2−xP2/C) hollow polyhedrons with tunable composition based on metal-organic frameworks (MOFs) template method. By the deliberate control of W doping, the synthesized catalyst with the composition of Co0.9W1.1P2/C is found to be able to achieve a current density of 10 mA·cm^(−2) at overpotentials of 35 and 54 mV in acidic and alkaline media, respectively. This combined electrochemical property stands atop the state-of-the-art electrocatalyst counterparts. To unveil the peculiar behavior of the structure, density functional theory (DFT) calculation was implemented and reveals that the surface W-doping facilitates the optimization of hydrogen absorption free energy (ΔGH*) as well as the thermodynamic and kinetics barriers for water dissociation, which is coupled with the hollow structure of Co-W phosphides, leading to the prominent HER catalytic performance.展开更多
基金This work was supported by the National Science Foundation for Young Scientists of China (No. 51901018)China Postdoctoral Science Foundation (No. 2019M660456)+4 种基金the National Natural Science Foundation of China (Nos. 51771027 and 21676216)Young Elite Scientists Sponsorship Program by China Association for Science and Technology (YESS, 2019QNRC001)the Fundamental Research Funds for the Central Universities (No. FRF-MP-19-001)National Key Research and Development Program of China (No. 2017YFB0702100)Singapore MOE AcRF Tier 1 grant M4011528.
文摘It has been of interest in seeking electrocatalysts that could exercise equally high-efficient and durable hydrogen evolution upon nonselective electrolytes in both acidic and alkaline environments. Herein, we report a facile strategy to fabricate cobalt tungsten phosphides (CoxW2−xP2/C) hollow polyhedrons with tunable composition based on metal-organic frameworks (MOFs) template method. By the deliberate control of W doping, the synthesized catalyst with the composition of Co0.9W1.1P2/C is found to be able to achieve a current density of 10 mA·cm^(−2) at overpotentials of 35 and 54 mV in acidic and alkaline media, respectively. This combined electrochemical property stands atop the state-of-the-art electrocatalyst counterparts. To unveil the peculiar behavior of the structure, density functional theory (DFT) calculation was implemented and reveals that the surface W-doping facilitates the optimization of hydrogen absorption free energy (ΔGH*) as well as the thermodynamic and kinetics barriers for water dissociation, which is coupled with the hollow structure of Co-W phosphides, leading to the prominent HER catalytic performance.
