The density functional theory(DFT)calculations have been performed to investigate the catalytic prop-erties of monolayer MoSi2N4 for hydrogen evolution reaction(HER).The DFT results show that similar to the majority of other two-dimensional(2D)materials,the pristine MoSi2N4 is inert for HER due to its weak affinity toward hydrogen,while monolayer MoSi2N4-x(x=0-0.25)exhibits the highly desirable HER catalytic activities by introducing surface nitrogen vacancy(NV).The predicted HER overpotential(0-60 mV)of monolayer MoSi2N4-x is lower than that(90 mV)of noble metal Pt,when the concentra-tion of surface NV is lower than 5.6％.Electronic structure calculations show that the spin-polarized states appear around the Fermi level after introducing surface NV,thus making the surface NV on 2D MoSi2N4 a quite suitable site for HER.Moreover,the HER activity of MoSi2N4-x is highly dependent on the surface NV concentration,which can be further related to the center of Si-3p band.Our results demonstrate that the newly discovered 2D MoSi2N4 can be served as a promising electrocatalyst for HER via appropriate defect engineering.

Wangwang Qian;Zhe Chen;Jinfeng Zhang;Lichang Yin

Shenyang National Laboratory for Materials Science,Institute of Metal Research,Chinese Academy of Sciences,Shenyang 110016,China;School of Materials Science and Engineering,University of Science and Technology of China,Shenyang 110016,China;Center of Artificial Photosynthesis for Solar Fuels,School of Science,Westlake University,Hangzhou 310024,China;Department of Physics and Electronic Information,Huaibei Normal University,Huaibei 235000,China

材料科学技术（英文版）

[1]Wangwang Qian;Zhe Chen;Jinfeng Zhang;Lichang Yin-.Monolayer MoSi2N4-x as promising electrocatalyst for hydrogen evolution reaction:A DFT prediction)[J].材料科学技术（英文版）,2022(04):215-222

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