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Dimethyl ether carbonylation to methyl acetate over highly crystalline zeolite-seed derived ferrierite

Abstract

Gas-phase carbonylation of dimethyl ether (DME) to methyl acetate (MA) was investigated on the ferrierite (FER) zeolite having different Si/Al molar ratios of 10.4 – 12.5 as well as high crystallinity synthesized by using various zeolite seed materials such as the MOR, ZSM-5 and USY. The enhanced crystallinity of the FER prepared by simply using the FER seed (denoted as FER@FER) having newly formed mesopore structures was responsible for an increased amount of the active Brønsted acid sites, which resulted in a higher MA productivity of 2.94 mmol/(gcat•h) with MA selectivity above 99%. The highly crystalline FER@FER revealed the suppressed depositions of aromatic coke precursors due to the less presence of defect sites. Compared to other zeolite seed-derived FER zeolites, the less amount of defect sites (extra-framework Lewis acidic Al species, EFAL) on the FER@FER was successfully controlled through a recrystallization process. The active Brønsted acid sites for DME carbonylation reaction were mainly originated from the preferential formations of the stable tetrahedral Al sites (especially, T2 sites of the Al-O-Si-O-Al framework of FER) on the 8 and 10-membered ring channels of the FER@FER. On those stable T2 sites having proper acid strengths, the adsorbed methyl intermediates formed by the dissociation of DME can be transformed to acetyl adsorbates by a relatively faster CO insertion rate on the vicinal Brønsted acid sites, which are resulted in a high catalytic stability and activity of the highly crystalline FER@FER.

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Publication details

The article was received on 14 Feb 2018, accepted on 11 May 2018 and first published on 14 May 2018


Article type: Paper
DOI: 10.1039/C8CY00329G
Citation: Catal. Sci. Technol., 2018, Accepted Manuscript
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    Dimethyl ether carbonylation to methyl acetate over highly crystalline zeolite-seed derived ferrierite

    J. Kim, H. Ham, H. S. Jung, Y. Wang, Y. He, N. Tsubaki, S. Cho, G. Y. Han and J. W. Bae, Catal. Sci. Technol., 2018, Accepted Manuscript , DOI: 10.1039/C8CY00329G

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