催化作用
异构化
化学
果糖
路易斯酸
介孔二氧化硅
布朗斯特德-洛瑞酸碱理论
介孔材料
选择性
有机化学
脱水
生物化学
作者
Tingwei Zhang,Haiying Wei,Yongcan Jin,Huining Xiao
标识
DOI:10.1016/j.cej.2022.140415
摘要
• A sulfonated Sn-containing dendritic mesoporous silica was designed and synthesized. • The modification of Sn-20DMS with -SO 3 H groups obviously increased the catalytic selectivity of HMF. • The recyclability of Sn-20DMS-SO 3 H for the dehydration of glucose was good. 5-Hydroxymethylfurfural (HMF) is a vital platform molecule for the synthesis of a wide variety of lignocellulosic-based biochemicals and biofuels. However, it is hard to prepare HMF from glucose, and a good match between the acid properties of the catalyst and the reaction requirements is necessary. Herein, Sn-doped dendritic mesoporous silica nanoparticles (Sn-xDMS) were synthesized through a simple in-situ co-assembly method. The uniform incorporation of Sn species onto the silica matrix created effective Lewis acid sites for the isomerization of glucose to fructose. Moreover, appropriately increasing the Sn loading amount was conducive to increasing the densities of Lewis acid sites. In the monophasic DMSO medium, the combination of Sn-20DMS and HCl could selectively catalyze the tandem reactions of the isomerization of glucose to fructose intermediate and the dehydration of fructose to HMF. Besides, acceptable HMF yields were also achieved when Sn-20DMS was used together with diluted H 2 SO 4 , sulfonated polymer, or sulfonated activated carbon. Due to the lack of suitable Brønsted acid sites, the catalytic performance of sole Sn-20DMS was much inferior to those of Brønsted acid catalyst-Sn-20DMS combinations. Therefore, the sulfonated Sn-20DMS (Sn-20DMS-SO 3 H) with enhanced Brønsted acidity was successfully prepared. Sn-20DMS-SO 3 H exhibited much higher catalytic selectivity toward HMF than Sn-20DMS. More importantly, the catalyst reuse experiment confirmed the good recyclability of Sn-20DMS-SO 3 H.
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