Tuning Binding Strength of Multiple Intermediates towards Efficient pH-universal Electrocatalytic Hydrogen Evolution by Mo8 O26 -NbNx Oy Heterocatalysts

Yang Yang; Lijia Liu; Shuai Chen; Wenjun Yan; Haiqing Zhou; Xian-Ming Zhang; Xiujun Fan

doi:10.1002/anie.202306896

Tuning Binding Strength of Multiple Intermediates towards Efficient pH-universal Electrocatalytic Hydrogen Evolution by Mo₈ O₂₆ -NbN_x O_y Heterocatalysts

Angew Chem Int Ed Engl. 2023 Nov 13;62(46):e202306896. doi: 10.1002/anie.202306896. Epub 2023 Oct 12.

Authors

Yang Yang^{1

2}, Lijia Liu³, Shuai Chen⁴, Wenjun Yan⁴, Haiqing Zhou⁵, Xian-Ming Zhang^{1

2}, Xiujun Fan^{2

6}

Affiliations

¹ College of Materials Science and Engineering, College of Chemistry, Key Laboratary of Interface Science and Engineering in Advanced Materials, Taiyuan University of Technology, Taiyuan, Shanxi, 030024, China.
² Institute of Crystalline Materials, Shanxi University, Taiyuan, Shanxi, 030006, China.
³ Department of Chemistry, University of Western Ontario, London, Ontario, N6 A 5B7, Canada.
⁴ State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, 030001, China.
⁵ Key Laboratory of Low-Dimensional Quantum Structures and Quantum Control of Ministry of Education, Department of Physics, Hunan Normal University, Changsha, 410081, China.
⁶ Engineering Research Center of Energy Storage Materials and Devices, Ministry of Education, School of Chemistry, Xi'an Jiaotong University, Xi An Shi, Xi'an, 710049, China.

PMID: 37747767
DOI: 10.1002/anie.202306896

Abstract

Developing efficient and robust hydrogen evolution reaction (HER) catalysts for scalable and sustainable hydrogen production through electrochemical water splitting is strategic and challenging. Herein, heterogeneous Mo₈ O₂₆ -NbN_x O_y supported on N-doped graphene (defined as Mo₈ O₂₆ -NbN_x O_y /NG) is synthesized by controllable hydrothermal reaction and nitridation process. The O-exposed Mo₈ O₂₆ clusters covalently confined on NbN_x O_y nanodomains provide a distinctive interface configuration and appropriate electronic structure, where fully exposed multiple active sites give excellent HER performance beyond commercial Pt/C catalyst in pH-universal electrolytes. Theoretical studies reveal that the Mo₈ O₂₆ -NbN_x O_y interface with electronic reconstruction affords near-optimal hydrogen adsorption energy and enhanced initial H₂ O adsorption. Furthermore, the terminal O atoms in Mo₈ O₂₆ clusters cooperate with Nb atoms to promote the initial H₂ O adsorption, and subsequently reduce the H₂ O dissociation energy, accelerating the entire HER kinetics.

Keywords: Electrocatalysis; Heterocatalysts; Hydrogen Evolution Reaction (HER); Mo8O26 Clusters; NbNxOy Nanodomains.

Abstract

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