Coral‐Biomimetic Structured Organic Electro‐Oxidations With Exceptional High‐Current Catalytic Performance

Abstract

ABSTRACT Organic electrooxidation reactions (OEORs) provide a thermodynamically favorable pathway for hydrogen production by replacing the oxygen evolution reaction with more readily oxidized organic substrates. However, the development of OEOR catalysts that simultaneously achieve high activity, stability, and energy efficiency at high current density remains a fundamental challenge. Herein, we report a bio‐inspired multiscale catalyst (CuxO@CuNiFeMoP/3D‐S) with a coral‐like hierarchical architecture, fabricated via integration of 3D‐printed triply periodic minimal surface scaffolds and pulse‐electrodeposited amorphous/crystalline heterostructures. This catalyst exhibits record‐breaking performance in the hydroxymethylfurfural oxidation reaction (HMFOR), requiring low potentials of 1.47 V at 500mA cm−2 and 1.57 V at 1000 mA cm−2 while maintaining 99.5% conversion. We identify a dual‐copper synergistic mechanism, where the coexistence of Cu+/Cu2+ together with Ni sites enables efficient catalysis under high current density. The mechanism demonstrates universality in diverse OEORs, especially achieving 500 mA cm−2 at 1.34 V for the urea oxidation reaction. By coupling OEORs with hydrogen evolution, this work provides an integrated architectural and mechanistic framework for designing multifunctional catalysts, enabling energy‐efficient hydrogen production with concurrent biomass valorization.