Glucose dehydration to 5-hydroxymethylfurfural on zirconium containing mesoporous MCM-41 silica catalysts
Glucose dehydration to 5-hydroxymethylfurfural on zirconium containing mesoporous MCM-41 silica catalysts
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DOI：
10.1016/j.fuel.2013.10.079
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发表时间：
2014-02-01
期刊：
影响因子：
7.4
通讯作者：
Maireles-Torres, P.
中科院分区：
文献类型：
--
作者：
Jimenez-Morales, I.;Santamaria-Gonzalez, J.;Maireles-Torres, P.
以介孔分子筛MCM-41为载体，负载ZrO 2，研究了葡萄糖在水/甲基异丁酮两相介质中选择性脱水制羟甲基糠醛（HMF）的反应。这些催化剂是：（a）在合成步骤中用Zr掺杂并在550和750 ℃活化的MCM-41二氧化硅，（B）用硫酸浸渍并在750 ℃活化的该固体，和（c）用硫酸锆浸渍并在750 ℃煅烧的MCM-41。所有这些催化剂都表现出酸性（282-563 μ mol的NH 3解吸g（1））和高表面积（359-635 m2 g（1）），在175 ℃和150分钟反应时间下葡萄糖脱水为HMF中具有活性。催化剂是相当有选择性的，因为只有果糖和HMF被检测到，而乙酰丙酸是不存在的。在合成凝胶（Zr-MCM-550）中将锆掺入MCM-41二氧化硅中后获得最具活性的催化剂，实现23%的HMF产率。此外，在500 ℃下煅烧2小时后，废催化剂的活性完全恢复。这些催化剂的TOF值在1.3和1.8 mmol HMF g（-1）h（-1）之间变化，催化性能与催化剂的酸性和结构特征良好相关。(C)2013爱思唯尔有限公司保留所有权利。
The selective dehydration of glucose to hydroxymethylfurfural (HMF) in a biphasic medium (water/methylisobuthylketone) has been studied by using different catalysts based on mesoporous MCM-41 silica containing ZrO2. These catalysts have been: (a) MCM-41 silica doped with Zr in the synthesis step and activated at 550 and 750 degrees C, (b) this solid impregnated with sulphuric acid and activated at 750 degrees C, and (c) MCM-41 impregnated with zirconium sulphate and calcined at 750 degrees C. All these catalysts exhibit acidic properties (282-563 mu mol of NH3 desorbed g (1)) and high surface areas (359-635 m(2) g (1)), being active in the dehydration of glucose to HMF at 175 degrees C and 150 min of reaction time. Catalysts are quite selective, since only fructose and HMF were detected, whereas levulinic acid was absent. The most active catalyst was obtained after incorporation of zirconium into a MCM-41 silica in the synthesis gel (Zr-MCM-550), achieving a HMF yield of 23%. Moreover, the activity of the spent catalyst is fully recovered after calcination at 500 degrees C during 2 h. TOF values of these catalysts vary between 1.3 and 1.8 mmol of HMF g(-1) h(-1), being the catalytic performance well correlated with the acidity and textural characteristics of catalysts. (C) 2013 Elsevier Ltd. All rights reserved.