期刊
JOURNAL OF CATALYSIS
卷 333, 期 -, 页码 207-216出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2015.10.013
关键词
Methyl lactate; Carbohydrate biomass; Mesoporous silica; Zr-SBA-15; Lewis acid
资金
- National Science Foundation [CBET 1337017]
- NSF through the MRSEC program
- Div Of Chem, Bioeng, Env, & Transp Sys
- Directorate For Engineering [1337017] Funding Source: National Science Foundation
The as-synthesized Zr-SBA-15 catalysts with tunable mesoporous structures showed excellent catalytic performance for the conversion of carbohydrates to methyl lactate in a one-pot process using near critical methanol or methanol-water mixture as the solvents. The effects of reaction conditions, including temperature, reaction time, and catalyst loading amount, on the conversions of carbohydrates and the yields of methyl lactate were investigated. The high yields of methyl lactate, up to 41% and 44%, were produced from pentose and hexose, respectively, in the near-critical methanol at 240 degrees C. Moreover, the Si/Zr ratio of the Zr-SBA-15 catalysts profoundly affected the Lewis acidity and therefore the catalytic activity and selectivity to methyl lactate in the conversion of carbohydrates. The pore size of the Zr-SBA-15 catalysts, tuned by the synthesis temperature, strongly affected the formation of solid residues. The key intermediates such as glyceraldehyde, glycolaldehyde, and pyruvaldehyde were used as probe reactants to understand the mechanism. The role of the Zr-SBA-15 catalyst in the aldol- and retro-aldol condensation, isomerization, and Cannizzaro reactions of carbohydrates and their derivatives was discussed. Furthermore, 28% and 27% yields of methyl lactate were obtained from cellulose and starch, respectively, in methanol-water mixture (5 wt% water and 95 wt% methanol) at 240 degrees C. The Zr-SBA-15 catalyst was relatively stable in short term without regeneration. (C) 2015 Elsevier Inc. All rights reserved.
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