Rapid synthesis of carbon quantum dot-integrated metal–organic framework nanosheets via electron beam irradiation for selective 5-hydroxymethylfurfural electrooxidation

Abstract

Balancing the adsorption of OH⁻ and 5-hydroxymethylfurfural (HMF) is crucial in optimizing the competing HMF oxidation reaction and oxygen evolution reaction, especially given the polymerization tendency of HMF in alkaline solutions. Herein, we present an innovative approach for rapidly synthesizing a NiFe bimetallic metal-organic framework (MOF) induced by electron-withdrawing carbon quantum dot (EW-CQD) via electron beam irradiation within 2 ​min. EW-CQD serve as structural regulators, expanding the NiFe-MOF interlayer spacing, increasing reactive site availability, and more effectively balancing the adsorption of OH⁻ and HMF, thereby significantly boosting the oxidation activity of HMF. The resulting EW-CQD-MOF exhibits a low potential of 1.36 ​V vs. RHE at 10 ​mA ​cm⁻² and maintains excellent durability over 120 ​h. Comprehensive in situ characterization elucidates the HMF oxidation reaction pathway, showing high selectivity towards 2,5-furandicarboxylic acid (FDCA) under ambient conditions, with an impressive HMF conversion rate of 94% and FDCA selectivity of 96% within 6 ​h. These findings underscore the critical role of structural optimization and adsorption balance in catalytic performance enhancement and offer valuable insights for designing high-efficiency catalysts, advancing sustainable catalytic processes.