Qianjia Ni , Mingwan Zhang , Bijun Tang , Weidong Hou , Kang Wang , Huazhang Guo , Jiye Zhang , Tao Han , Minghong Wu , Liang Wang
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引用次数: 0
摘要
平衡OH -和5-羟甲基糠醛(HMF)的吸附对于优化HMF氧化反应和析氧反应是至关重要的,特别是考虑到HMF在碱性溶液中的聚合倾向。本文提出了一种利用电子束辐照在2 min内快速合成吸电子碳量子点(EW-CQD)诱导的NiFe双金属金属有机骨架(MOF)的创新方法。EW-CQD作为结构调节剂,扩大了nfe - mof层间距,增加了活性位点的可用性,更有效地平衡了OH -和HMF的吸附,从而显著提高了HMF的氧化活性。所得到的EW-CQD-MOF在10 mA cm⁻2时表现出1.36 V的低电位,并在120小时内保持良好的耐久性。全面的原位表征阐明了HMF氧化反应途径,在环境条件下对2,5-呋喃二羧酸(FDCA)具有很高的选择性,在6 h内HMF的转化率为94%,FDCA的选择性为96%。这些发现强调了结构优化和吸附平衡在提高催化性能中的重要作用,并为设计高效催化剂、推进可持续催化过程提供了有价值的见解。
Rapid synthesis of carbon quantum dot-integrated metal–organic framework nanosheets via electron beam irradiation for selective 5-hydroxymethylfurfural electrooxidation
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.