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Nano Research 2024, 17(3): 1232-1241 https://doi.org/10.1007/s12274-023-6011-5
Research Article | Issue | Published: 23 August 2023

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

Show Author's Information 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
Keywords:
hydrogen evolution activity, complementary multisite catalysts, sequential reactive water management, interfacial water molecules
Topics:
Electrolysis
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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Abstract Full text Electronic supplementary material About this article

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.


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Abstract
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Electronic supplementary material
About this article

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

Show Author's information 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

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 activity, complementary multisite catalysts, sequential reactive water management, interfacial water molecules

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Publication history
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Acknowledgements

Publication history

Received: 26 June 2023
Revised: 13 July 2023
Accepted: 15 July 2023
Published: 23 August 2023
Issue date: March 2024

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

We acknowledge technical support from the Analytical and Testing Center at Huazhong University of Science and Technology.

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