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Direct Synthesis of 2,5-Diformylfuran from Carbohydrates Using High-Silica MOR Zeolite-Supported Isolated Vanadium Species
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2017-10-05 00:00:00 , DOI: 10.1021/acssuschemeng.7b02002
Wei Zhang 1 , Tongsuo Meng 1 , Junjie Tang 1 , Wenxia Zhuang 1 , Yu Zhou 1 , Jun Wang 1
Affiliation  

Directly transforming carbohydrates into high value-added chemicals provides an economic and sustainable path for the utilization of the renewable biomass resource. Herein, we fabricated an efficient catalytic system for the straightforward conversion of various carbohydrates into 2,5-diformylfuran (DFF) by using vanadium oxide supported on high-silica mordenite (MOR) zeolites in the presence of hydrochloric acid. The synthesis of high-silica MOR zeolites was achieved in a template-free dense system featuring energy savings and environmental friendliness, delivering the SiO2/Al2O3 ratio up to 80. The conversion of fructose into DFF reached a high yield of 96.0% in a one-pot and one-step reaction by oxidation with atmospheric O2 (balloon), with facile recovery and good reusability of the catalyst. Good yields were also obtained in the direct synthesis of DFF from other carbohydrates including glucose, sucrose, inulin, raffinose, maltose, and starch. The high performance relied on the unique high-silica MOR skeleton, which (1) endowed the highly dispersed V species mainly in the form of isolated tetrahedrally coordinated [V2O8]6– species as the active oxidative sites and (2) provided satisfactory acidity for the formation of intermediate 5-hydroxymethylfurfural (HMF) and sufficient resistance to corrosion under an acid environment for good stability.

中文翻译:

使用高硅MOR沸石负载分离钒物种从碳水化合物直接合成2,5-二甲酰呋喃

直接将碳水化合物转化为高附加值的化学品,为利用可再生生物质资源提供了经济和可持续的途径。在这里,我们制造了一种高效的催化系统,用于在盐酸存在下,通过负载在高二氧化硅丝光沸石(MOR)沸石上的氧化钒,将各种碳水化合物直接转化为2,5-二甲酰呋喃(DFF)。高二氧化硅MOR沸石的合成是在无模板的致密系统中实现的,该系统具有节能和环境友好的特点,将SiO 2 / Al 2 O 3的比例提高到80。果糖向DFF的转化率高达96.0一锅一步反应,通过与大气O 2的氧化反应得到的%(气球),具有容易回收和良好的催化剂可重复使用性。从其他碳水化合物(包括葡萄糖,蔗糖,菊粉,棉子糖,麦芽糖和淀粉)直接合成DFF时,也获得了良好的收率。高性能依赖于独特的高二氧化硅MOR骨架,(1)赋予了高度分散的V物种,其主要形式为孤立的四面体配位的[V 2 O 8 ] 6–物种作为活性氧化位点,而(2)提供了具有令人满意的酸度,可形成中间体5-羟甲基糠醛(HMF),并且在酸性环境下具有足够的耐腐蚀性,从而具有良好的稳定性。
更新日期:2017-10-05
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