Two‐Dimensional Porous Molybdenum Phosphide/Nitride Heterojunction Nanosheets for pH‐Universal Hydrogen Evolution Reaction

Herein, we present a new strategy for the synthesis of 2D porous MoP/Mo 2 N heterojunction nanosheets based on the pyrolysis of 2D [PMo 12 O 40 ] 3− ‐melamine (PMo 12 ‐MA) nanosheet precursor from a polyethylene glycol (PEG)‐mediated assembly route. The heterostructure nanosheets are ca. 20 nm thick and have plentiful pores (<5 nm). These structure features offer advantages to promote the HER activity, including the favorable water dissociation kinetics around heterojunction as confirmed by theoretical calculations, large accessible surface of 2D nanosheets, and enhanced mass‐transport ability by pores. Consequently, the 2D porous MoP/Mo 2 N heterojunction nanosheets exhibit excellent HER activity with low overpotentials of 89, 91 and 89 mV to achieve a current density of 10 mA cm −2 in alkaline, neutral and acidic electrolytes, respectively. The HER performance is superior to the commercial Pt/C at a current density >55 mA cm −2 in neutral medium and >190 mA cm −2 in alkaline medium.