Activating Surface Oxygen in Ce/Mo‐Doped Ni Oxyhydroxide for Synergistically Enhancing Furfural Oxidation and Hydrogen Evolution at Ampere‐Level Current Densities

Abstract The integration of biomass‐platform molecule oxidation with water electrolysis is a promising strategy to reduce energy consumption in hydrogen production and obtain high‐value chemicals simultaneously, yet the efficiency of organic oxidation requires further improvement. Herein, we developed a highly efficient Ce, Mo co‐doped Ni‐based (oxy)hydroxide catalyst, where Mo with high spin state promotes the adsorption of furfural (FA), while Ce activates surface lattice oxygen (O L ), lowering the energy barrier for O L ─OH coupling to form OOH, the key intermediate for high current densities. The catalyst achieves an industrial‐grade current density of 1000 mA cm − 2 at a remarkably low potential of 1.46 V versus RHE in furfural oxidation, with exceptional selectivity (99.4%) and Faradaic efficiency (97.7%) for furoic acid. When deployed as anode in an anion‐exchange membrane reactor, the NiMoCe/NF catalyst sustains a current density of 500 and 1000 mA cm − 2 at a cell voltage of only 1.85 and 2.15 V, respectively, surpassing most reported continuous flow electrolyzers limited to 200 mA cm − 2 . Moreover, the system exhibits outstanding durability after 200 h of continuous operation. This work provides critical insights into the rational design of catalysts for energy‐efficient biomass valorization coupled with industrial hydrogen production.