期刊
APPLIED CATALYSIS A-GENERAL
卷 618, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcata.2021.118122
关键词
Asymmetric ether; Cyclopentyl methyl ether; Cyclopentanol; Zeolite catalysts; Gas-phase
资金
- Grant Agency of Slovakia [APVV-17-0302]
- Ministry of Education, Science, Research and Sport of the Slovak Republic [VEGA 1/0808/18]
- Czech Science Foundation [19-27551X, 20-12099S]
An efficient zeolite-catalyzed one-step synthesis of valuable asymmetric cyclopentyl methyl ether (CPME) was developed using ZSM-5 catalysts with high selectivity and yield. Decreasing Si/Al ratios in ZSM-5 improves conversion without affecting selectivity. FTIR studies suggest a Rideal-Eley mechanism for the advertisement of reactants in ZSM-5.
Symmetric ethers can be synthesized through the acid-catalyzed self-etherification of biomass-derived alcohols. However, synthesis of asymmetric ethers via catalytic cross-etherification of alcohols is limited by poor selectivity. Herein, we developed an efficient zeolite-catalyzed one-step synthesis of valuable asymmetric cyclopentyl methyl ether (CPME) using gas-phase reaction of bio-based cyclopentanol and methanol. Among different medium- (FER, MCM-22, ZSM-5) and large-pore (BEA, MOR, USY) aluminosilicate zeolites, commercial ZSM-5 catalysts with 2D system of intersecting channels are markedly more selective to CPME. The targeted CPME was produced with a selectivity of 83 % and a yield higher than 80 % over the ZSM-5 catalysts with Si/Al ratios ranging from 15 to 40. Decrease in Si/Al ratio in ZSM-5 enhanced the conversion value, while not affecting the selectivity. FTIR study of the step-by-step adsorption of both reactants in ZSM-5 evidenced the Rideal-Eley mechanism with cyclopentanol adsorbed on acid sites. Therefore, heterogeneously catalyzed gas-phase crossetherification of renewable cyclopentanol and methanol is a promising process for large-scale applications thanks to its mild operating conditions, high yields and selectivity when using commercial ZSM-5 zeolites as catalysts.
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