Construction of N‐Doped Carbon Nanotube Confining MoC/Ni Mott–Schottky Heterojunction on Porous Carbonized Wood for Efficient Urea‐Assisted Water Splitting

Abstract Exploring highly efficient and cost‐effective electrocatalysts for urea electrolysis is crucial for advancing water‐cycle‐related catalytic processes/devices. Herein, the natural wood is converted into a series of MoC/Ni@NCNT/CWs monolithic chainmail electrocatalysts, in which MoC coupling Ni nanoparticles encapsulated within N‐doped carbon nanotubes (NCNTs) are in situ constructed on porous carbonized wood (CW). Such 3D hierarchical structure with super‐hydrophilic property is beneficial for mass/electron transfer during electrochemical reactions and enhances corrosion resistance. Density functional theory (DFT) calculations and X‐ray photoelectron spectroscopy (XPS) reveal the strong interfacial interaction and optimized electron redistribution within the MoC/Ni Mott–Schottky heterojunction. When employed as a self‐standing electrode in an alkaline electrolyte, the MoC/Ni@NCNT/CW‐1 exhibits ultralow potential of 1.319 and 1.358 V vs. RHE at 10 and 100 mA cm ⁻² for urea oxidation reaction (UOR), respectively. Interestingly, the surface‐active center Ni ³⁺ ‐O is reconstructed during the UOR. Moreover, the MoC/Ni@NCNT/CW‐1 as a bifunctional catalyst for urea‐assisted water splitting can reach 50 mA cm ⁻² at only 1.63 V and operate stably over 48 h. Such design of wood‐derived chainmail electrode offers a promising strategy for developing robust electrocatalysts combined with the high‐value utilization of forestry residuals.