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

(2020) NATURE MATERIALS. 19(10). p.1081-1087
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Abstract
The methanol-to-hydrocarbons reaction on zeolites produces olefins from many sources, but catalyst stability is a major challenge. Here, by combining operando measurements and simulations, the formation and identification of deactivating carbonaceous species throughout the reaction are achieved. 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.
Keywords
Mechanical Engineering, General Materials Science, Mechanics of Materials, General Chemistry, Condensed Matter Physics, TO-OLEFINS CONVERSION, RAMAN-SPECTROSCOPY, REACTION TEMPERATURE, REACTION-MECHANISM, DIMETHYL ETHER, COKE FORMATION, ZEOLITES, H-ZSM-5, SAPO-34, FLUORESCENCE

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MLA
Lezcano-Gonzalez, I., et al. “Insight into the Effects of Confined Hydrocarbon Species on the Lifetime of Methanol Conversion Catalysts.” NATURE MATERIALS, vol. 19, no. 10, 2020, pp. 1081–87, doi:10.1038/s41563-020-0800-y.
APA
Lezcano-Gonzalez, I., Campbell, E., Hoffman, A., Bocus, M., Sazanovich, I. V., Towrie, M., … Beale, A. M. (2020). Insight into the effects of confined hydrocarbon species on the lifetime of methanol conversion catalysts. NATURE MATERIALS, 19(10), 1081–1087. https://doi.org/10.1038/s41563-020-0800-y
Chicago author-date
Lezcano-Gonzalez, I., E. Campbell, Alexander Hoffman, Massimo Bocus, I. V. Sazanovich, M. Towrie, M. Agote-Aran, et al. 2020. “Insight into the Effects of Confined Hydrocarbon Species on the Lifetime of Methanol Conversion Catalysts.” NATURE MATERIALS 19 (10): 1081–87. https://doi.org/10.1038/s41563-020-0800-y.
Chicago author-date (all authors)
Lezcano-Gonzalez, I., E. Campbell, Alexander Hoffman, Massimo Bocus, I. V. Sazanovich, M. Towrie, M. Agote-Aran, E. K. Gibson, A. Greenaway, Kristof De Wispelaere, Veronique Van Speybroeck, and A. M. Beale. 2020. “Insight into the Effects of Confined Hydrocarbon Species on the Lifetime of Methanol Conversion Catalysts.” NATURE MATERIALS 19 (10): 1081–1087. doi:10.1038/s41563-020-0800-y.
Vancouver
1.
Lezcano-Gonzalez I, Campbell E, Hoffman A, Bocus M, Sazanovich IV, Towrie M, et al. Insight into the effects of confined hydrocarbon species on the lifetime of methanol conversion catalysts. NATURE MATERIALS. 2020;19(10):1081–7.
IEEE
[1]
I. Lezcano-Gonzalez et al., “Insight into the effects of confined hydrocarbon species on the lifetime of methanol conversion catalysts,” NATURE MATERIALS, vol. 19, no. 10, pp. 1081–1087, 2020.
@article{8678627,
  abstract     = {{The methanol-to-hydrocarbons reaction on zeolites produces olefins from many sources, but catalyst stability is a major challenge. Here, by combining operando measurements and simulations, the formation and identification of deactivating carbonaceous species throughout the reaction are achieved.

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.}},
  author       = {{Lezcano-Gonzalez, I. and Campbell, E. and Hoffman, Alexander and Bocus, Massimo and Sazanovich, I. V. and Towrie, M. and Agote-Aran, M. and Gibson, E. K. and Greenaway, A. and De Wispelaere, Kristof and Van Speybroeck, Veronique and Beale, A. M.}},
  issn         = {{1476-1122}},
  journal      = {{NATURE MATERIALS}},
  keywords     = {{Mechanical Engineering,General Materials Science,Mechanics of Materials,General Chemistry,Condensed Matter Physics,TO-OLEFINS CONVERSION,RAMAN-SPECTROSCOPY,REACTION TEMPERATURE,REACTION-MECHANISM,DIMETHYL ETHER,COKE FORMATION,ZEOLITES,H-ZSM-5,SAPO-34,FLUORESCENCE}},
  language     = {{eng}},
  number       = {{10}},
  pages        = {{1081--1087}},
  title        = {{Insight into the effects of confined hydrocarbon species on the lifetime of methanol conversion catalysts}},
  url          = {{http://dx.doi.org/10.1038/s41563-020-0800-y}},
  volume       = {{19}},
  year         = {{2020}},
}

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