Directional Construction of Vertical Nitrogen‐Doped 1T‐2H MoSe₂/Graphene Shell/Core Nanoflake Arrays for Efficient Hydrogen Evolution Reaction

The low utilization of active sites and sluggish reaction kinetics of MoSe₂ severely impede its commercial application as electrocatalyst for hydrogen evolution reaction (HER). To address these two issues, the first example of introducing 1T MoSe₂ and N dopant into vertical 2H MoSe₂ /graphene shell/core nanoflake arrays that remarkably boost their HER activity is herein described. By means of the improved conductivity, rich catalytic active sites and highly accessible surface area as a result of the introduction of 1T MoSe₂ and N doping as well as the unique structural features, the N-doped 1T-2H MoSe₂ /graphene (N-MoSe₂ /VG) shell/core nanoflake arrays show substantially enhanced HER activity. Remarkably, the N-MoSe₂ /VG nanoflakes exhibit a relatively low onset potential of 45 mV and overpotential of 98 mV (vs RHE) at 10 mA cm⁻² with excellent long-term stability (no decay after 20 000 cycles), outperforming most of the recently reported Mo-based electrocatalysts. The success of improving the electrochemical performance via the introduction of 1T phase and N dopant offers new opportunities in the development of high-performance MoSe₂ -based electrodes for other energy-related applications.