Ni₃S₂/Co₉S₈ embedded poor crystallinity NiCo layered double hydroxides hierarchical nanostructures for efficient overall water splitting

Nickel–cobalt bimetallic layered double hydroxides (NiCo LDHs) are potential electrocatalysts with high performance and stability for overall water-splitting. However, its weak conductivity limits its practical applications. Herein, a simple hydrothermal in-situ conversion strategy is employed for constructing the novel heterogeneous electrocatalyst of Ni₃S₂/Co₉S₈ embedded poor crystallinity (Pc) NiCo LDH nanosheet arrays grown on the Ni foam (Pc-NiCo LDH/ Ni₃S₂/Co₉S₈), which can improve the conductivity via regulating the crystallinity. The crystallinity of NiCo LDH is well regulated by adjusting the amount of sulfur source, and the construction of Ni₃S₂/Co₉S₈ heterostructure exposes more active sites, improves the electrical conductivity, enhances the electronic interaction between NiCo LDH and Ni₃S₂/Co₉S₈, and significantly promotes the kinetics of water splitting. The optimized Pc-NiCo LDH/Ni₃S₂/Co₉S₈ hierarchical structure as both the anode and cathode exhibit the overall water splitting performance with the cell voltage of only 1.744 V to achieve the current density of 50 mA cm⁻² in the alkaline media and shows the competitive H₂ and O₂ production rate of 6.4 and 3.1 μL s⁻¹, respectively, suggesting its potential practical applications. This work provides a novel idea for the design of multiphase composite electrocatalysts applied in water splitting.