Insight into the effects of confined hydrocarbon species on the lifetime of methanol conversion catalysts.
Journal
Nature materials
ISSN: 1476-4660
Titre abrégé: Nat Mater
Pays: England
ID NLM: 101155473
Informations de publication
Date de publication:
10 2020
10 2020
Historique:
received:
27
09
2019
accepted:
11
08
2020
pubmed:
16
9
2020
medline:
16
9
2020
entrez:
15
9
2020
Statut:
ppublish
Résumé
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.
Identifiants
pubmed: 32929250
doi: 10.1038/s41563-020-0800-y
pii: 10.1038/s41563-020-0800-y
doi:
Types de publication
Journal Article
Research Support, Non-U.S. Gov't
Langues
eng
Sous-ensembles de citation
IM
Pagination
1081-1087Références
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