期刊
APPLIED CATALYSIS A-GENERAL
卷 526, 期 -, 页码 62-69出版社
ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcata.2016.07.025
关键词
Levulinic acid; Angelica lactone; Silanol; Vapor-phase lactonization; Reaction equilibrium
资金
- JST, Strategic International Collaborative Research Program, SICORP
Vapor-phase lactonization of levulinic acid to produce angelica lactones, which include alpha-, beta- and gamma-form isomers, was performed in fixed-bed down-flow glass reactors over various oxide catalysts. SiO2 and SiO2-Al2O3 showed relatively high catalytic activity. The lactonization of levulinic acid to angelica lactones was found to be an endothermic equilibrium reaction, and the pressure equilibrium constant was calculated to be 0.2 atm at 275 degrees C. High temperatures and reduced pressures were effective for shifting the equilibrium from levulinic acid to angelica lactones, while the suitable reaction temperature was estimated to be 275 degrees C because temperatures higher than 275 degrees C decreased the selectivity to angelica lactones. The highest angelica lactones yield of 87.5% was achieved at a levulinic acid conversion of 95.3% over SiO2 under reduced pressure conditions of ca. 5 kPa at 275 degrees C. IR, NH3-TPD and TG analyses were performed for characterizing the catalysts used after the reactions together with a silylated SiO2 prepared for studying the active species on SiO2. The silanol groups of SiO2 with weak acidity were proposed to be the active species. (C) 2016 Elsevier B.V. All rights reserved.
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