Anion-cation dual-doping strategy induced electronic structure regulation of sulfide to enhance hydrogen evolution...

Large-scale deployment of water splitting for hydrogen generation urgently demands the sustainable and scalable fabrication of inexpensive, effective, and durable electrocatalysts capable of operating effectively at industrial-level current density. Herein, we present an innovative electrocatalyst by incorporating Mo and P into CoS₂ lattices formed over carbonized wood (referred to as Mo, P-CoS₂/CW). This self-supported electrode, with its hierarchically porous framework, significantly enhances the exposure of active surface sites and promotes mass transfer during the hydrogen evolution reaction (HER). Experimental results and density functional theory (DFT)-based calculations reveal that co-incorporating of Mo and P can modify local charge density of active sites, accelerates electron transfer, enhance conductivity, and optimizes adsorption energy of hydrogen species, collectively promoting the HER. Additionally, the abundant porosity among stacked units facilitates the efficient electrolyte infiltration and the sliding of hydrogen bubbles, ensuring rapid electrolyte recharging and bubble release during high-current catalysis. Accordingly, the Mo, P-CoS₂/CW electrode can serve as a durable electrocatalyst for HER, achieving an industrial-level current density of 1000 mA cm^-2 at a low overpotential of 289 mV. This binder-free electrode also demonstrates exceptional stability for 100 h. This research offers a novel approach to designing catalysts for energy storage and conversion utilizing sustainable wood-based materials.