Progressive steps and catalytic cycles in methanol-to-hydrocarbons reaction over acidic zeolites  

作　　者：Liu Yang Chang Wang Weili Dai Guangjun Wu Naijia Guan Landong Li 

机构地区：[1]a School of Materials Science and Engineering,Nankai University,Tianjin 300350,China [2]Frontiers Science Center for New Organic Matter and Key Laboratory of Advanced Energy Materials Chemistry of Ministry of Education,College of Chemistry,Nankai University,Tianjin 300071,China

出　　处：《Fundamental Research》2022年第2期184-192,共9页自然科学基础研究（英文版）

基　　金：This work was supported by the National Natural Science Foundation of China(Grants No.21972069,22025203);the Fundamental Research Funds for the Central Universities,and Frontiers Science Center for New Organic Matter,Nankai University(Grant No.63181206).

摘　　要：Understanding the complete reaction network and mechanism of methanol to-hydrocarbons remains a key chal-lenge in the field of zeolite catalysis and C1 chemistry.Inspired by the identification of the reactive surface methoxy species on solid acids,several direct mechanisms associated with the formation of the first C-C bond in methanol conversion have been recently disclosed.Identifying the stepwise involvement of the initial intermedi-ates containing the first CC bond in the whole reaction process of methanol to-hydrocarbons conversion becomes possible and attractive for the further development of this important reaction.Herein,several initial unsaturated aldehydes/ketones containing the C-C bond are identified via complementary spectroscopic techniques.With the combination of kinetic and spectroscopic analyses,a complete roadmap of the zeolite catalyzed methanol-to-hydrocarbons conversion from the initial CC bonds to the hydrocarbon pool species via the oxygen-containing unsaturated intermediates is clearly ilustrated.With the participation of both Bronsted and Lewis acid sites in H-ZSM-5 zeolite,an initial aldol-cycle is proposed,which can be closely connected to the well-known dual-cycle mechanism in the methanol-to-hydrocarbons conversion.

关 键 词：METHANOL-TO-HYDROCARBONS H-ZSM-5 zeolite Reaction mechanism First carbon-carbon bond Aldol-cycle 

分 类 号：TQ426[化学工程]