Huang, J; Wang, J; Xie, R; Tian, Z; Chai, G; Zhang, Y; Lai, F; ... Brett, DJL; + view all Huang, J; Wang, J; Xie, R; Tian, Z; Chai, G; Zhang, Y; Lai, F; He, G; Liu, C; Liu, T; Shearing, PR; Brett, DJL; - view fewer (2020) A universal pH range and a highly efficient Mo2C-based electrocatalyst for the hydrogen evolution reaction. Journal of Materials Chemistry A 10.1039/d0ta07091b.

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Abstract

Electrochemical water splitting is a promising approach to generate ‘green’ hydrogen. The efficiency of this process relies on the effectiveness of the electrocatalysts used. The electro-kinetics of the hydrogen evolution reaction (HER) is highly pH dependent and conventional catalysts typically are expensive and rare platinum-based materials. The development of low-cost, multi-component electrocatalysts, where each of the components has a synergistic effect, can be an effective approach to improve kinetics. Herein, a series of transition metal (Fe, Mn, Co, and Ni)-modified molybdenum carbides in a nitrogen-doped carbon matrix (TM-Mo2C@NCF) are synthesised to maximise exposed active sites. Among them, Fe-Mo2C@NCF delivers the best-in-class HER performance over a wide range of electrolytes. Tafel slopes of 76, 109 and 110 mV dec−1 and overpotentials of 65, 130 and 129 mV at 10 mA cm−2 were obtained in 1.0 M KOH, 1.0 M phosphate buffer solution (PBS) and 0.5 M H2SO4, respectively. The computational study further indicates that the synergistic electronic modulation co-activated by Fe and N dopants in Fe-Mo2C@NCF can reduce the Gibbs free energy of H adsorption (ΔGH*) and render the Mo–Mo bridge site the most energetically favorable adsorption site for the H* intermediate, which contributes to an increased HER performance.

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