Insight into the effects of confined hydrocarbon species on the lifetime of methanol conversion catalysts

alexander — Tue, 15 Sep 2020 08:47:31 +0000

I. Lezcano-Gonzalez, E. Campbell, A.E.J. Hoffman, M. Bocus, I.V. Sazanovich, M. Towrie, M. Agote-Aran, E.K. Gibson, A. Greenaway, K. De Wispelaere, V. Van Speybroeck, A.M. Beale

Nature Materials

19, 1081–1087

2020

Abstract

The methanol-to-hydrocarbons reaction refers collectively to a series of important industrial catalytic processes to produce either olefins or gasoline. Mechanistically, methanol conversion proceeds through a ‘pool’ of hydrocarbon species. For the methanol-to-olefins process, these species can be delineated broadly into ‘desired’ lighter olefins and ‘undesired’ heavier fractions that cause deactivation in a matter of hours. The crux in further catalyst optimization is the ability to follow the formation of carbonaceous species during operation. Here, we report the combined results of an operando Kerr-gated Raman spectroscopic study with state-of-the-art operando molecular simulations, which allowed us to follow the formation of hydrocarbon species at various stages of methanol conversion. Polyenes are identified as crucial intermediates towards formation of polycyclic aromatic hydrocarbons, with their fate determined largely by the zeolite topology. Notably, we provide the missing link between active and deactivating species, which allows us to propose potential design rules for future-generation catalysts.

DOI

http://dx.doi.org/10.1038/s41563-020-0800-y

Private attachment

NatMater.pdf

Operando Raman spectroscopy to pinpoint the onset of deactivation in zeolites

alexander — Thu, 17 Mar 2022 13:10:47 +0000

A.E.J. Hoffman, I. Lezcano-Gonzalez, E. Campbell, M. Bocus, I.V. Sazanovich, M. Towrie, A.M. Beale, V. Van Speybroeck

ISBN/ISSN:

Poster

Conference / event / venue

FEZA 2021

online

Monday, 5 July, 2021 to Friday, 9 July, 2021

Operando Raman spectroscopy to pinpoint the onset of deactivation in zeolites

alexander — Mon, 01 Mar 2021 15:14:00 +0000

A.E.J. Hoffman, I. Lezcano-Gonzalez, E. Campbell, M. Bocus, I.V. Sazanovich, M. Towrie, A.M. Beale, V. Van Speybroeck

ISBN/ISSN:

Talk

Conference / event / venue

The Netherlands' Catalysis and Chemistry Conference

online

Monday, 1 March, 2021

Abstract (private)

Abstract_submitted.pdf

Center for Molecular Modeling - M. Towrie

Insight into the effects of confined hydrocarbon species on the lifetime of methanol conversion catalysts

Abstract

DOI

Private attachment

Operando Raman spectroscopy to pinpoint the onset of deactivation in zeolites

Conference / event / venue

Operando Raman spectroscopy to pinpoint the onset of deactivation in zeolites

Conference / event / venue

Abstract (private)