Abstract
Highlights
A strongly coupled platinum/molybdenum nitrides nanocluster heterostructure has been prepared by using Pt-containing Anderson-type polyoxometalates as precursors.
The pronounced electronic coupling at the Pt/Mo2N cluster interface facilitates the catalytic decomposition of H2O through synergistic stabilization of Pt-H* and Mo-OH*.
The optimized Pt/Mo2N-NrGO exhibits a remarkably low overpotential, high mass activity, and exceptional long-term durability (>500 h at 1500 mA cm-2) in a practical anion-exchange membrane water electrolyzer.
Creating strongly coupled heterostructures with favorable catalytic activities is crucial for promoting the performance of catalytic reactions, especially those involve multiple intermediates. Herein, we fabricated a strongly coupled platinum/molybdenum nitrides nanocluster heterostructure on nitrogen-doped reduced graphene oxide (Pt/Mo₂N–NrGO) for alkaline hydrogen evolution reaction. The well-defined Pt-containing Anderson-type polyoxometalates promote strong interfacial Pt–N–Mo bonding in Pt/Mo2N–NrGO, which exhibits a remarkably low overpotential, high mass activity, and exceptional long-term durability (> 500 h at 1500 mA cm⁻2) in an anion-exchange membrane water electrolyzer (AEMWE). Operando Raman spectroscopy and density functional theory reveal that pronounced electronic coupling at the Pt/Mo₂N cluster interface facilitates the catalytic decomposition of H2O through synergistic stabilization of intermediates (Pt–H* and Mo-OH*), thereby enhancing the kinetics of the rate-determining Volmer step. Techno-economic analysis indicates a levelized hydrogen production cost of $2.02 kg⁻1, meeting the US DOE targets. Our strategy presents a viable pathway to designing next-generation catalysts for industrial AEMWE for green hydrogen production.
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1 China University of Petroleum (East China), State Key Laboratory of Chemical Safety, Shandong Key Laboratory of Intelligent Energy Materials, School of Materials Science and Engineering, Qingdao, People’s Republic of China (GRID:grid.497420.c) (ISNI:0000 0004 1798 1132); Zhangjiang Institute for Advanced Study, Shanghai Jiao Tong University, State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Future Material Innovation Center, Shanghai, People’s Republic of China (GRID:grid.16821.3c) (ISNI:0000 0004 0368 8293)
2 China University of Petroleum (East China), State Key Laboratory of Chemical Safety, Shandong Key Laboratory of Intelligent Energy Materials, School of Materials Science and Engineering, Qingdao, People’s Republic of China (GRID:grid.497420.c) (ISNI:0000 0004 1798 1132)
3 Zhangjiang Institute for Advanced Study, Shanghai Jiao Tong University, State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Future Material Innovation Center, Shanghai, People’s Republic of China (GRID:grid.16821.3c) (ISNI:0000 0004 0368 8293)
4 Qingdao Binhai University, School of Mechanical and Electronic Engineering, Qingdao, People’s Republic of China (GRID:grid.449394.7) (ISNI:0000 0004 8348 9867)
5 Institute of Materials, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Science, Fuzhou, People’s Republic of China (GRID:grid.418036.8) (ISNI:0000 0004 1793 3165)
6 San Diego State University, Department of Chemistry and Biochemistry, San Diego, USA (GRID:grid.263081.e) (ISNI:0000 0001 0790 1491)
7 China University of Petroleum (East China), State Key Laboratory of Chemical Safety, Shandong Key Laboratory of Intelligent Energy Materials, School of Materials Science and Engineering, Qingdao, People’s Republic of China (GRID:grid.497420.c) (ISNI:0000 0004 1798 1132); Hefei Comprehensive National Science Center, Institute of Energy, Hefei, People’s Republic of China (GRID:grid.513034.0)