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Surface enhanced dynamic nuclear polarization solid-state NMR spectroscopy sheds light on Brønsted–Lewis acid synergy during the zeolite catalyzed methanol-to-hydrocarbon process

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Abstract

After a prolonged effort over two decades, the reaction mechanism of the zeolite-catalyzed methanol-to-hydrocarbon (MTH) process is now well-understood: the so-called ‘direct mechanism’ (via direct coupling of two methanol molecules) is responsible for the formation of the initial carbon–carbon bonds, while the hydrocarbon pool (HCP)-based dual cycle mechanism is responsible for the formation of reaction products. While most of the reaction events occur at zeolite Brønsted acid sites, the addition of Lewis acid sites (i.e., via the introduction of alkaline earth cations like calcium) has been shown to inhibit the formation of deactivating coke species and hence increase the catalyst lifetime. With the aim to have an in-depth mechanistic understanding, herein, we employ magic angle spinning surface-enhanced dynamic nuclear polarization solid-state NMR spectroscopy to illustrate that the inclusion of Lewis acidity prevents the formation of carbene/ylide species on the zeolite, directly affecting the equilibrium between arene and olefin cycles of the HCP mechanism and hence regulating the ultimate product selectivity and catalyst lifetime.

Graphical abstract: Surface enhanced dynamic nuclear polarization solid-state NMR spectroscopy sheds light on Brønsted–Lewis acid synergy during the zeolite catalyzed methanol-to-hydrocarbon process

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Publication details

The article was received on 07 May 2019, accepted on 20 Aug 2019 and first published on 21 Aug 2019


Article type: Edge Article
DOI: 10.1039/C9SC02215E
Chem. Sci., 2019, Advance Article
  • Open access: Creative Commons BY-NC license
    All publication charges for this article have been paid for by the Royal Society of Chemistry

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    Surface enhanced dynamic nuclear polarization solid-state NMR spectroscopy sheds light on Brønsted–Lewis acid synergy during the zeolite catalyzed methanol-to-hydrocarbon process

    A. Dutta Chowdhury, I. Yarulina, E. Abou-Hamad, A. Gurinov and J. Gascon, Chem. Sci., 2019, Advance Article , DOI: 10.1039/C9SC02215E

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