Free-standing phosphorous-doped molybdenum nitride in 3D carbon nanosheet towards hydrogen evolution

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Highly efficient electrocatalysts towards hydrogen evolution reaction (HER) with large current density at all-pH values are critical for the sustainable hydrogen production.Herein,we report a free-standing HER electrode,phosphorous-doped molybdenum nitride nanoparticles embedded in 3-dimentional carbon nanosheet matrix (P-Mo2N-CNS) fabricated via one-step carbonization and in-situ formation.The asprepared catalyst shows free-standing architecture with interconnected porous microstructure.P-doped Mo2N nanoparticles with an average diameter of 4.4 nm are well embedded in the 3-dimentional vertical carbon nanosheets matrix.Remarkable electrocatalytic HER performance is observed in alkaline,neutral and acidic media at large current densities.The overpotential of P-Mo2N-CNS to drive a current density of 100 mA cm-2 in 0.5 M H2SO4 and 1.0 M PBS is only 181 and 221 mV,respectively.In particular,the current density reaches up to 1000 mA cm-2 at a low overpotential of 256 mV in 1.0 M KOH,much better than that of the commercial Pt/C catalyst.Density functional theory calculations suggest the optimized H sorption kinetics on Mo2N after P doping,elucidating the superior activity.
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