Mechanistic Insight into Ethanol Dehydration over SAPO-34 Zeolite by Solid-state NMR Spectroscopy
作者机构：National Centre for Magnetic Resonance in WuhanState Key Laboratory of Magnetic Resonance and Atomic and Molecular PhysicsWuhan Institute of Physics and MathematicsInnovation Academy for Precision Measurement Science and TechnologyChinese Academy of SciencesWuhan 430071P.R.China
出 版 物：《Chemical Research in Chinese Universities》 (高等学校化学研究（英文版）)
年 卷 期：2022年第38卷第1期
页 面：155-160页
核心收录：
学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学]
基 金：This work was supported by the National Natural Science Foundation of China (Nos.22072165,U1932218,21991092,21733013,21773296) the National Natural Science Foundation of China-Royal Society(No.22061130202) the Project of the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2021329)
主 题：Ethanol dehydration SAPO-34 Intermediate Reaction mechanism Solid-state NMR
摘 要：The reaction mechanism of ethanol dehydration over SAPO-34 zeolite is investigated by using solid-state NMR spectroscopy. SAPO-34 zeolites with different Si contents are prepared and their acidities are characterized by NMR experiments. The higher content of stronger Brønsted acid sites is correlated to the higher Si content. The adsorption of ethanol on the Brønsted acid sites in SAPO-34 leads to the formation of frustrated Lewis pairs(FLPs). Surface ethoxy species is observed by the dehydration of the FLP sites at room temperature, which can be further converted into ethene products. The decomposing of diethyl ether over Brønsted acid sites is responsible for the formation of ethoxy species at higher reaction temperatures. Triethyloxonium ions are formed in the reaction. A plausible reaction mechanism is proposed for the dehydration of ethanol over SAPO-34.
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