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Research Article

Sequential reactant water management by complementary multisite catalysts for surpassing platinum hydrogen evolution activity

Yu Lin1, Defang Ding1, Shicheng Zhu2, Qunlei Wen2, Huangjingwei Li2, Zhen Li1, Youwen Liu2( ), Yi Shen1( )
China Engineering Research Center of Nano-Geomaterials of Ministry of Education, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, China
State Key Laboratory of Materials Processing and Die & Mould Technology, and School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
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Graphical Abstract

We proposed a multisite complementary strategy that incorporates hydrophilic Mo and electrophilic V into Ni-based catalysts to divide the distinct steps on atomically dispersive sites and thus realize sequential regulation of the HER process. By management of reactive H2O molecules, the NiMoV oxides multisite catalysts surpass Pt/C hydrogen evolution activity (49 mV@10 mA∙cm−2 over 140 h).

Abstract

Alkaline hydrogen evolution reaction (HER) offers a near-zero-emission approach to advance hydrogen energy. However, the activity limited by the multiple reaction steps involving H2O molecules transfer, absorption, and activation still unqualified the thresholds of economic viability. Herein, we proposed a multisite complementary strategy that incorporates hydrophilic Mo and electrophilic V into Ni-based catalysts to divide the distinct steps on atomically dispersive sites and thus realize sequential regulation of the HER process. The Isotopic labeled in situ Raman spectroscopy describes 4-coordinated hydrogen bonded H2O to be free H2O passing the inner Helmholtz plane in the vicinity of the catalysts under the action of hydrophilic Mo sites. Furthermore, potential-dependent electrochemical impedance spectroscopy (EIS) reveals that electrophilic V sites with abundant 3d empty orbitals could activate the lone-pair electrons in the free H2O molecules to produce more protic hydrogen, and dimerize into H2 at the Ni sites. By the sequential management of reactive H2O molecules, NiMoV oxides multisite catalysts surpass Pt/C hydrogen evolution activity (49 mV@10 mA∙cm−2 over 140 h). Profoundly, this study provides a tangible model to deepen the comprehension of the catalyst–electrolyte interface and create efficient catalysts for diverse reactions.

Keywords

hydrogen evolution activitycomplementary multisite catalystssequential reactive water managementinterfacial water molecules

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Nano Research
Volume 17 Issue 3,
March 2024
Pages 1232-1241
DOI: 10.1007/s12274-023-6011-5
Cite this article:
Lin Y, Ding D, Zhu S, et al. Sequential reactant water management by complementary multisite catalysts for surpassing platinum hydrogen evolution activity. Nano Research, 2024, 17(3): 1232-1241. https://doi.org/10.1007/s12274-023-6011-5
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Received: 26 June 2023
Revised: 13 July 2023
Accepted: 15 July 2023
Published: 23 August 2023
© Tsinghua University Press 2023
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