A universal pH range and a highly efficient Mo2C-based electrocatalyst for the hydrogen evolution reaction

Jiajia Huang; Jingyi Wang; Ruikuan Xie; Zhihong Tian; Guoliang Chai; Yanwu Zhang; Feili Lai; Guanjie He; Chuntai Liu; Tianxi Liu; Paul R. Shearing; Dan J. L. Brett

doi:10.1039/D0TA07091B

A universal pH range and a highly efficient Mo₂C-based electrocatalyst for the hydrogen evolution reaction†

Jiajia Huang,

^a Jingyi Wang,^a Ruikuan Xie,^d Zhihong Tian,*^c Guoliang Chai,

^d Yanwu Zhang,

^a Feili Lai,

^e Guanjie He,

*^bf Chuntai Liu,^c Tianxi Liu,^c Paul R. Shearing

^b and Dan J. L. Brett

^b

Author affiliations

* Corresponding authors

^a School of Chemical Engineering, Zhengzhou University, Zhengzhou 450001, P. R. China

^b Electrochemical Innovation Lab, Department of Chemical Engineering, University College London, London WC1E 7JE, UK
E-mail: g.he@ucl.ac.uk

^c Key Laboratory of Materials Processing and Mold (Zhengzhou University), Ministry of Education, National Engineering Research Center for Advanced Polymer Processing Technology, Zhengzhou University, Zhengzhou, Henan 450002, China
E-mail: zhihong.tian@zzu.edu.cn

^d State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences (CAS), Fuzhou, 350002 Fujian, P. R. China

^e Department of Chemistry, KU Leuven, Celestijnenlaan 200F, Leuven 3001, Belgium

^f School of Chemistry, University of Lincoln, Joseph Banks Laboratories, Green Lane, Lincoln, UK

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 (ΔG_H^*) and render the Mo–Mo bridge site the most energetically favorable adsorption site for the H* intermediate, which contributes to an increased HER performance.

Journal of Materials Chemistry A

A universal pH range and a highly efficient Mo₂C-based electrocatalyst for the hydrogen evolution reaction†

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A universal pH range and a highly efficient Mo₂C-based electrocatalyst for the hydrogen evolution reaction

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Journal of Materials Chemistry A