Engineering Metallic Heterostructure Based on Ni3 N and 2M-MoS2 for Alkaline Water Electrolysis with Industry-Compatible Current Density and Stability

Abstract

Alkaline water electrolysis is commercially desirable to realize large-scale hydrogen production. Although nonprecious catalysts exhibit high electrocatalytic activity at low current density (10-50 mA cm^-2 ), it is still challenging to achieve industrially required current density over 500 mA cm^-2 due to inefficient electron transport and competitive adsorption between hydroxyl and water. Herein, the authors design a novel metallic heterostructure based on nickel nitride and monoclinic molybdenum disulfide (Ni₃ N@2M-MoS₂ ) for extraordinary water electrolysis. The Ni₃ N@2M-MoS₂ composite with heterointerface provides two kinds of separated reaction sites to overcome the steric hindrance of competitive hydroxyl/water adsorption. The kinetically decoupled hydroxyl/water adsorption/dissociation and metallic conductivity of Ni₃ N@2M-MoS₂ enable hydrogen production from Ni₃ N and oxygen evolution from the heterointerface at large current density. The metallic heterostructure is proved to be imperative for the stabilization and activation of Ni₃ N@2M-MoS₂ , which can efficiently regulate the active electronic states of Ni/N atoms around the Fermi-level through the charge transfer between the active atoms of Ni₃ N and MoMo bonds of 2M-MoS₂ to boost overall water splitting. The Ni₃ N@2M-MoS₂ incorporated water electrolyzer requires ultralow cell voltage of 1.644 V@1000 mA cm^-2 with ≈100% retention over 300 h, far exceeding the commercial Pt/C║RuO₂ (2.41 V@1000 mA cm^-2 , 100 h, 58.2%).

Keywords: active electronic states; alkaline water electrolysis; interface engineering; large current density; metallic heterostructures.