Porous Mo2C−MoP Heterostructure on Carbon Cloth for Efficient Hydrogen Evolution Reaction over a Broad pH Range

Heterogeneous structure composed of different active materials is an important strategy to improve the HER performance of catalysts, due to the synergistic effects on the interface. Here, we synthesized a Mo2C−MoP heterostructure by phosphating porous β‐Mo2C nanostructures with red phosphorus powder. XRD, Raman, XPS, SEM and TEM results suggested that Mo2C−MoP heterostructure with porous nanostructures were obtained on carbon cloth at 550 °C (MoCP‐550), which showed remarkable HER activity over a broad pH range. A low η10 of 51 mV and a small Tafel slope of 56.7 mV dec−1 was achieved in 1.0 M KOH, and a low η10 of 82 mV and a small Tafel slope of 49.8 mV dec−1 in 0.5 M H2SO4. MoCP‐550 also exhibited excellent electrocatalytic stability in both alkaline and acidic electrolytes. Density functional theory (DFT) calculations identified that Mo2C−MoP heterostructure has more suitable H* adsorption free energy compared to pure Mo2C and pure MoP. Catalytic cloth: Mo2C−MoP heterostructure was prepared by phosphating porous β‐Mo2C nanostructures, which shows excellent catalytic hydrogen evolution performance. DFT calculation showed more suitable ΔGH* for Mo2C−MoP heterostructure than Mo2C and MoP.