Phase reconstruction and electronic coupling interactions of Ni(OH)₂/P-doped 2D MoS₂ heterostructures for low-voltage water splitting and high-performance zinc-air batteries

Developing efficient, low-cost, and durable catalysts for water-splitting and zinc-air batteries is crucial to advancing clean energy technologies. In this study, we present a novel heterostructure of α-Ni(OH)₂ and phosphorus-doped MoS₂ supported on carbon cloth (Ni(OH)₂/P-MoS₂/CC) engineered through synergistic valence tuning and phase manipulation to enhance the performance of hydrogen (HER) and oxygen evolution reactions (OER). The heterostructure exhibits a reduced operating voltage of 1.42 V at 10 mA cm⁻² in 1.0 M KOH, outperforming recently reported literature with remarkable durability over 330 h, thereby surpassing the performances of commercial Pt-C and IrO₂. X-ray absorption near-edge structure analysis confirms high-valence Ni (IV) as the active phase. The catalyst demonstrates enhanced stability for seawater, supported by Cl⁻ anions. Density functional theory calculations reveal an increased electron density and electron charge transfer from the P dopant to the substrates, which is attributed to heterostructure engineering. The optimized d-band center effectively balances adsorption and desorption energies, significantly lowering the Gibbs free energy barrier for both HER and OER. The catalyst achieves high power density and exceptional cycling stability over 3600 cycles in zinc-air battery applications, underscoring its potential for energy applications.