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Heterojunction Mo-based binary and ternary nitride catalysts with Pt-like activity for the hydrogen evolution reaction

Xueling Wang,Xuming Zhang,Yifan Xu,Hao Song,Xingrui Min,Zihuan Tang,Chaoran Pi,Jianping Li,Biao Gao,Yang Zheng,Xiang Peng,Paul K. Chu,Kaifu Huo

The development of earth-abundant electrocatalysts with Pt-like catalytic activity for the hydrogen evolution reaction (HER) is of great significance to green hydrogen production . Herein, a novel strategy is described to construct dual-phase nitride nanobelts composed of Mo 2 N and Ni 0.2 Mo 0.8 N by nitridation of Ni 2+ intercalated layered MoO 3 nanobelts (NBs). The Mo 2 N/Ni 0.2 Mo 0.8 N catalyst exhibits superior stability and a low overpotential of 26 mV at 10 mA cm −2 and Tafel slope of 31 mV dec −1 in both the alkaline electrolyte and simulated seawater, which is comparable to or better than that of the benchmark Pt/C catalyst. The excellent alkaline HER characteristics is attributed to the Mo 2 N/Ni 0.2 Mo 0.8 N heterostructure with adjustable content and robust interfaces and without metal Ni segregation and structure collapse during nitridation. Density-functional theory (DFT) calculations and experiments reveal that the Mo 2 N/Ni 0.2 Mo 0.8 N interface with strong electronic interactions optimizes H adsorption/desorption yielding moderately weak bonding metal sites with positive ΔG H* as the catalytic centers, thereby accelerating the HER kinetics and boosting the HER activity. The results reveal a simple strategy for the preparation of heterostructured nitride-based catalysts with Pt-like activity for hydrogen evolution.