School of Chemistry and Chemical Engineering, Nanchang University, No. 999 Xuefu Avenue, Nanchang, 330031, P. R. China.
School of Chemical Engineering and Technology, Tianjin University, No.92 Weijin Road, Tianjin, 300072, P. R. China.
Angew Chem Int Ed Engl. 2022 Aug 22;61(34):e202205453. doi: 10.1002/anie.202205453. Epub 2022 Jul 13.
One pot synthesis of 2,5-dimethylfuran (2,5-DMF) from saccharides under mild conditions is of importance for the production of biofuel and fine chemicals. However, the synthesis requires a multitude of active sites and suffers from slow kinetics due to poor diffusion in most composite catalysts. Herein, a metal-acid functionalized 2D metal-organic framework (MOF; Pd/NUS-SO H), as an ultrathin nanosheet of 3-4 nm with Lewis acid, Brønsted acid, and metal active sites, was prepared based on the diazo method for acid modification and subsequent metal loading. This new composite catalyst gives substantially higher yields of DMF than all reported catalysts for different saccharides (fructose, glucose, cellobiose, sucrose, and inulins). Characterization suggests that a cascade of reactions including polysaccharide hydrolysis, isomerization, dehydration, and hydrodeoxygenation takes place with rapid molecular interactions.
在温和条件下，从糖合成 2,5-二甲基呋喃（2,5-DMF）对于生物燃料和精细化学品的生产具有重要意义。然而，由于大多数复合催化剂中扩散性差，该合成需要大量的活性位，并且动力学较慢。在此，通过重氮法进行酸改性和随后的金属负载，制备了一种金属-酸功能化二维金属有机骨架（MOF；Pd/NUS-SO H），其作为具有路易斯酸、布朗斯台德酸和金属活性位的 3-4nm 超薄纳米片。与不同糖（果糖、葡萄糖、纤维二糖、蔗糖和菊粉）的所有报道的催化剂相比，这种新型复合催化剂使 DMF 的产率大大提高。表征表明，包括多糖水解、异构化、脱水和加氢脱氧在内的级联反应伴随着快速的分子相互作用发生。
