分子筛拓扑结构对甲缩醛羰基化影响的反应机理研究

doi:10.19964/j.issn.1006-4990.2024-0204

Abstract

Abstract:

Dimethoxymethane（DMM） carbonylation over zeolites to methyl methoxyacetate（MMAc） is currently one of the most promising C1 chemical reactions for both fundamental research and industrialization.Zeolite topology influences DMM carbonylation evidently.In this work，zeolites with different topology including MFI，MOR and FAU were chosen to compare their DMM carbonylation activity and selectivity.As the increase of reaction space，both DMM carbonylation activity and selectivity were increased gradually.The improved DMM carbonylation selectivity could be attributed to the inhibition of DMM disproportionation and DMM carbonylation activity was rate⁃limited by both the generation and conversion of acyl intermediate.The low conversion kinetics conditions test excluding the influence of diffusion revealed that DMM carbonylation activity for FAU was about 9 times higher than that for MFI.Methoxy acetyl intermediate over MFI and FAU in the process of DMM carbonylation was directly observed by in⁃situ IR，and the relative intensity of carbonylation acyl and disproportionation acyl was positive to DMM carbonylation selectivity.Finally，a possible DMM carbonylation and disproportionation mechanism over zeolites was proposed and a DMM carbonylation kinetic formula was deduced based on the in⁃situ IR results and the understanding of the reaction mechanism.

Key words: carbonylation reaction, dimethoxymethane, zeolite, in?situ IR, kinetic

CLC Number:

TQ426.6

GAO Shaolei, WANG Yingli, QI Liang. Mechanism study on influence of zeolite topology on dimethoxymethane carbonylation reaction[J]. Inorganic Chemicals Industry, 2025, 57(5): 71-78.

Figures/Tables 8

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References 32

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Mechanism study on influence of zeolite topology on dimethoxymethane carbonylation reaction

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