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Issue 16, 2019
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Mechanistic role of water in HSSZ-13 catalyzed methanol-to-olefins conversion

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Abstract

Co-feeding water leads to a simultaneous attenuation of chain initiation and chain termination rates in HSSZ-13 catalyzed methanol-to-olefins (MTO) conversion. Density functional theory calculations and transient stoichiometric experiments support the plausibility of formaldehyde hydrolysis occurring over zeolitic Brønsted acid sites at MTO-relevant temperatures. A monotonic decrease in MTO chain initiation and termination rates, and a concurrent monotonic increase in total turnovers as a function of water co-feed partial pressure are consistent with the occurrence and mechanistic relevance of formaldehyde hydrolysis effected by co-fed water. Initiation/termination rates and total turnovers normalized by their corresponding values in the absence of water co-feeds at the same temperature show the expected trends as a function of reaction temperature, assuming equilibrium between formaldehyde and methanediol. These results underscore the implications of formaldehyde hydrolysis chemistry when assessing the mechanistic role of water in methanol-to-olefins conversion specifically, and deactivation mechanisms in zeolite-catalyzed hydrocarbon conversion processes more generally.

Graphical abstract: Mechanistic role of water in HSSZ-13 catalyzed methanol-to-olefins conversion

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Supplementary files

Article information


Submitted
24 May 2019
Accepted
14 Jul 2019
First published
24 Jul 2019

Catal. Sci. Technol., 2019,9, 4374-4383
Article type
Paper
Author version available

Mechanistic role of water in HSSZ-13 catalyzed methanol-to-olefins conversion

P. Bollini, T. T. Chen, M. Neurock and A. Bhan, Catal. Sci. Technol., 2019, 9, 4374
DOI: 10.1039/C9CY01015G

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