Lezcano-Gonzalez, I;
Campbell, E;
Hoffman, AEJ;
Bocus, M;
Sazanovich, IV;
Towrie, M;
Agote-Aran, M;
... Beale, AM; + view all
(2020)
Insight into the effects of confined hydrocarbon species on the lifetime of methanol conversion catalysts.
Nature Materials
, 19
pp. 1081-1087.
10.1038/s41563-020-0800-y.
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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.
| Type: | Article |
|---|---|
| Title: | Insight into the effects of confined hydrocarbon species on the lifetime of methanol conversion catalysts |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1038/s41563-020-0800-y |
| Publisher version: | https://doi.org/10.1038/s41563-020-0800-y |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | Heterogeneous catalysis, Porous materials, Raman spectroscopy, Reaction mechanisms |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10112481 |
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