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

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 chemical 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 furfural, while Ce activates surface lattice oxygen (OL), lowering the energy barrier for OL‐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 vs. 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 hours of continuous operation. This work provides critical insights into the rational design of catalysts for energy‐efficient biomass valorization coupled with industrial hydrogen production.