Acid-Functionalized SBA-15-Type Periodic Mesoporous Organosilicas and Their Use in the Continuous Production of 5-Hydroxymethylfurfural
Acid-Functionalized SBA-15-Type Periodic Mesoporous Organosilicas and Their Use in the Continuous Production of 5-Hydroxymethylfurfural
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DOI：
10.1021/cs300303v
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发表时间：
2012-07
期刊：
影响因子：
12.9
通讯作者：
M. Tucker;Anthony J. Crisci;B. Wigington;Neelay M. Phadke;R. Alamillo;Jin-ping Zhang;S. Scott;J. Dumesic
中科院分区：
文献类型：
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作者：
M. Tucker;Anthony J. Crisci;B. Wigington;Neelay M. Phadke;R. Alamillo;Jin-ping Zhang;S. Scott;J. Dumesic
在四氢呋喃和水（4:1 w/w）的单相溶液中，用果糖连续制备5-羟甲基糠醛（HMF）的管式反应器中，对几种负载型酸催化剂的活性、选择性和稳定性进行了评价。填充固体催化剂的反应器在403 K下长时间运行至190 h。比较了三种丙基磺酸功能化的有序多孔二氧化硅（一种无机sba -15型二氧化硅和两种乙烷桥接的sba -15型有机二氧化硅）与丙基磺酸改性的无序多孔二氧化硅的行为。具有有序孔结构的催化剂的HMF选择性在60% ~ 75%之间，而在相同反应条件下，无序孔结构的催化剂的选择性最高为20%。后者也是最不稳定的，失活的一级速率常数为0.152 h-1。有机硅具有较好的水热稳定性和较长时间的稳定催化活性。
The activity, selectivity, and stability of several supported acid catalysts were evaluated in tubular reactors designed to produce 5-hydroxymethylfurfural (HMF) continuously from fructose dissolved in a single-phase solution of THF and H2O (4:1 w/w). The reactors, packed with the solid catalysts, were operated at 403 K for extended periods, up to 190 h. The behaviors of three propylsulfonic acid-functionalized, ordered porous silicas (one inorganic SBA-15-type silica, and two ethane-bridged SBA-15-type organosilicas) were compared with that of a propylsulfonic acid-modified, nonordered, porous silica. The HMF selectivity of the catalysts with ordered pore structures ranged from 60 to 75%, whereas the selectivity of the nonordered catalyst under the same reaction conditions peaked at 20%. The latter was also the least stable, deactivating with a first-order rate constant of 0.152 h–1. The organosilicas are more hydrothermally stable and maintained a steady catalytic activity longer than the inorganic SBA-...