High-Entropy Regulation of Lattice Oxygen p-Band toward Sustainable Electrocatalytic Biomass Valorization

Electrocatalytic 5-hydroxymethylfurfural oxidation reaction (HMFOR) presents a promising approach for converting biomass derivatives into high-value chemicals but is challenging due to poor stability and low Faradaic efficiency. Herein, we present a high-entropy NiCoFeMnAl layer double hydroxide (NiCoFeMnAl-LDH) for HMFOR via a hydrothermal method. At a potential of 1.43 V vs RHE, the process demonstrates exceptional performance with 100% HMF conversion, 99.09% selectivity for 2,5-furandicarboxylic acid (FDCA), and Faradaic efficiency of 96.9%, which outperform the majority of previously reported state-of-the-art electrocatalysts. The impressive performance is primarily attributed to the high-entropy surface chemical environment that regulates the p-band center of lattice oxygen, thereby reducing the Gibbs free energy of the rate-determining step and accelerating the kinetics of charge transfer. Moreover, NiCoFeMnAl-LDH significantly mitigates the common issue of carbon deposition observed in traditional LDH-based materials, thereby enhancing the stability for HMFOR. The tuning of the lattice oxygen p-band center provides valuable insights for the design of high-performance electrocatalysts.