Amorphization Engineering Coupled with Anion Leaching Boosts Precatalyst Reconstruction for Enhanced Urea Oxidation

Abstract Ni‐based materials have emerged as a class of promising precatalysts for the urea oxidation reaction (UOR), yet inherent structure‐related reconstruction behavior of the precatalyst and correlation with electrocatalytic activity are not well‐understood, severely hindering rational design of advanced catalysts. Herein, a new type of precatalyst, amorphous Mn‐incorporated NiWO₄ (a‐MnNi‐WO₄), is constructed via rapid co‐precipitation followed by mild heat treatment, and proposed for expediting the UOR. Intriguingly, loose and flexible amorphous phase engineering and leachable WO₄²⁻ incorporation can collaboratively prompt a‐MnNi‐WO₄ to access fast and complete self‐reconstruction during UOR, thus generating porous, oxygen‐vacancy‐enriched, and low‐crystalline Mn‐doped NiOOH with optimized electronic structure for prompting urea adsorption and the rate‐determining step of ^*COO desorption. Impressively, the a‐MnNi‐WO₄ can deliver admirable UOR behavior and considerably outperform the crystalline counterpart as well as the amorphous ones without WO₄²⁻ or Mn species incorporation, favorably presenting the state‐of‐the‐art level. This work elucidates an in‐depth understanding of the reconstruction ability of the precatalyst for promoting the UOR, and material design principle for achieving fast and deep self‐reconstruction via amorphization engineering and sacrificial anion etching is expected to extend to construct other advanced electrocatalytic systems.