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Experimental Evidence on the Formation of Ethene through Carbocations in Methanol Conversion over H‐ZSM‐5 Zeolite
Authors:Chao Wang  Xianfeng Yi  Prof Dr Jun Xu  Dr Guodong Qi  Pan Gao  Weiyu Wang  Dr Yueying Chu  Dr Qiang Wang  Dr Ningdong Feng  Dr Xiaolong Liu  Dr Anmin Zheng  Prof Dr Feng Deng
Affiliation:National Center for Magnetic Resonance in Wuhan, State Key Laboratory Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathmatics, Chinese Academy of Sciences, Wuhan 430071 (P.R. China)
Abstract:The methanol to olefins conversion over zeolite catalysts is a commercialized process to produce light olefins like ethene and propene but its mechanism is not well understood. We herein investigated the formation of ethene in the methanol to olefins reaction over the H‐ZSM‐5 zeolite. Three types of ethylcyclopentenyl carbocations, that is, the 1‐methyl‐3‐ethylcyclopentenyl, the 1,4‐dimethyl‐3‐ethylcyclopentenyl, and the 1,5‐dimethyl‐3‐ethylcyclopentenyl cation were unambiguously identified under working conditions by both solid‐state and liquid‐state NMR spectroscopy as well as GC‐MS analysis. These carbocations were found to be well correlated to ethene and lower methylbenzenes (xylene and trimethylbenzene). An aromatics‐based paring route provides rationale for the transformation of lower methylbenzenes to ethene through ethylcyclopentenyl cations as the key hydrocarbon‐pool intermediates.
Keywords:carbocations  olefins  reaction mechanisms  solid‐state NMR spectroscopy  zeolites
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