Surface Reconstruction‐Engineered Transition Metals Composite Nanosheets for Green and High‐Efficiency Electrocatalytic Conversion of Biomass‐Derived HMF to FDCA

Abstract The electrocatalytic oxidation of 5‐hydroxymethylfurfural (HMF) to 2,5‐furandicarboxylic acid (FDCA), a sustainable alternative to petroleum‐derived polymers, is limited by high energy demands and precious‐metal reliance. This work presents a cost‐effective Ni‐Co PTA nanosheet electrocatalyst fabricated via electrodeposition, solvothermal treatment, and in situ activation. Unlike conventional Au/Pd‐based catalysts or transition metal hydroxides, the activated catalyst features ultrathin hexagonal nanosheets with enriched Ni 3 ⁺/Co 3 ⁺ species, achieving 99.9% conversion and high FDCA yield at 0.35 V(vs. HgO/Hg), outperforming non‐precious benchmarks and approaching noble metals. Mechanistic analysis reveals that alkaline cycling drives evolution from dense hydroxide precursors into nanosheets., enlarging the electrochemical surface area and reducing charge‐transfer resistance. XPS and in situ Raman spectroscopy confirm Ni 2 ⁺→Ni 3 ⁺/Co 2 ⁺→Co 3 ⁺ transitions, enabling NiOOH formation at lower potentials. Notably, the catalyst exhibits versatile oxidation activity toward glycerol, urea, and methanol, while maintaining high yield under practical concentrations. This work provides a scalable and sustainable strategy for biomass valorization, bridging the gap between non‐precious catalyst design and industrial feasibility for green chemical synthesis.