Hydrothermally Stable, Conformal, Sulfated Zirconia Monolayer Catalysts for Glucose Conversion to 5-HMF

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• 作者：Amin Osatiashtiani ; Adam F. Lee ; Marta Granollers ; D. Robert Brown ; Luca Olivi ; Gabriel Morales ; Juan A. Melero ; Karen Wilson
• 刊名：ACS Catalysis
• 出版年：2015
• 出版时间：July 2, 2015
• 年：2015
• 卷：5
• 期：7
• 页码：4345-4352
• 全文大小：433K
• ISSN：2155-5435

文摘

The grafting and sulfation of zirconia conformal monolayers on SBA-15 to create mesoporous catalysts of tunable solid acid/base character is reported. Conformal zirconia and sulfated zirconia (SZ) materials exhibit both Br枚nsted and Lewis acidity, with the Br枚nsted/Lewis acid ratio increasing with film thickness and sulfate content. Grafted zirconia films also exhibit amphoteric character, whose Br枚nsted/Lewis acid site ratio increases with sulfate loading at the expense of base sites. Bilayer ZrO₂/SBA-15 affords an ordered mesoporous material with a high acid site loading upon sulfation and excellent hydrothermal stability. Catalytic performance of SZ/SBA-15 was explored in the aqueous phase conversion of glucose to 5-HMF, delivering a 3-fold enhancement in 5-HMF productivity over nonporous SZ counterparts. The coexistence of accessible solid basic/Lewis acid and Br枚nsted acid sites in grafted SZ/SBA-15 promotes the respective isomerization of glucose to fructose and dehydration of reactively formed fructose to the desired 5-HMF platform chemical.