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Formation of HCO+ ion by protonation of carbon monoxide in zeolites: the origin of catalytic activity in methanol carbonylation

30 July 2021, Version 1
Working Paper
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

We show that CO can be protonated by Brønsted acid sites to form the super-electrophilic HCO+ cation in H-zeolites such as mordenite. This reactivity stems from the confining environment of small 8-ring side pockets of H-MOR. HCO+ is a catalytically active super-electrophile: it carbonylates dimethyl ether and hydrocarbons to methyl acetate and aldehydes.

Keywords

carbon monoxide protonation
zeolite
methanol and dimethyl ether carbonylation
carbon monoxide CO chemistry in zeolites

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Version History

Jul 30, 2021 Version 1

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The content is available under CC BY NC ND 4.0 [opens in a new tab]

DOI

10.26434/chemrxiv-2021-lpb2g
D O I: 10.26434/chemrxiv-2021-lpb2g [opens in a new tab]

Funding

The research described in paper is part of the Quickstarter Initiative at Pacific Northwest National Laboratory. It was conducted under the Laboratory Directed Research and Development Program at PNNL, a multiprogram national laboratory operated by Battelle for the U.S. Department of Energy (DOE) under Contract DE-AC05-76RL01830. The research described in this paper was performed in the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the DOE's Office of Biological and Environmental Research. This work was supported by US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Biosciences, and Geosciences.

Author’s competing interest statement

The author(s) have declared they have no conflict of interest with regard to this content

Ethics

The author(s) have declared ethics committee/IRB approval is not relevant to this content

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