Abstract
Electrocatalytic water splitting is the most directly available route to generate renewable and sustainable hydrogen.Here,we report the design of a composite material in which arrays of square pillar-like NiMoO4 nanorods coated with N,P-doped carbon layers are uniformly contained in numerous nested nanoparti-cle structures.The catalysts have superior catalytic activity,requiring only 59 mV and 187 mV for HER and OER to attain a current density of 10mA/cm2,respectively.The assembled two-electrode electrolytic cell required a voltage of 1.48 V to reach 10mA/cm2,along with excellent long-term stability.Theoretical cal-culations reveal that electrons aggregate and redistribute at the heterogeneous interface,with the d-band centers of the Ni and Fe atoms being positively shifted compared to the Fermi level,effectively optimiz-ing the adsorption of intermediates and reducing the Gibbs free energy,thus accelerating the catalytic process.Meanwhile,an integrated solar-driven water-splitting system demonstrated a high and stable solar-to-hydrogen efficiency of 18.20%.This work provides new possibilities for developing non-precious metal-based bifunctional electrocatalysts for large-scale water splitting applications.