The effects of MTG catalysis on methanol mobility in ZSM-5

S. K. Matam, A J O'Malley, C R A Catlow, Suwardiyanto, P Collier, A P Hawkins, Andrea Zachariou, David Lennon, I P Silverwood, S F Parker, R F Howe

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Abstract

We analyse the dynamics of methanol in ZSM-5 catalysts both with and without the hydrocarbon pool, resulting from the methanol to gasoline (MTG) reaction taking place at 623 K and 673 K for three days, to determine the effects of catalyst use on molecular mobility. Using quasielastic neutron scattering (QENS), we observe that methanol is immobile on the QENS instrumental time scale in the fresh catalyst (ZSM-5-F) and in the sample used to convert methanol for 3 days at 623 K (ZSM-5-623). However, in zeolite ZSM-5-673 (MTG at 673 K for 3 days) we observe isotropic methanol rotation with an immobile fraction of 0.58 and a rotational diffusion coefficient of DR = 3 × 1010 s−1. The observed differences between the zeolites in methanol dynamics are attributed to the development of mesoporosity in ZSM-5-673 due to the high reaction temperature of 673 K, leading to dislodgement of lattice Al as is evident from NMR data.
Original languageEnglish
Pages (from-to)3304-3312
Number of pages9
JournalCatalysis Science & Technology
Volume8
Issue number13
Early online date12 Jun 2018
DOIs
Publication statusPublished - 2018

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Catalysis
Gasoline
Methanol
Neutron scattering
Catalysts
Zeolites
Hydrocarbons
Nuclear magnetic resonance

Cite this

Matam, S. K., O'Malley, A. J., Catlow, C. R. A., Suwardiyanto, Collier, P., Hawkins, A. P., ... Howe, R. F. (2018). The effects of MTG catalysis on methanol mobility in ZSM-5. Catalysis Science & Technology, 8(13), 3304-3312. https://doi.org/10.1039/C8CY00422F

The effects of MTG catalysis on methanol mobility in ZSM-5. / Matam, S. K.; O'Malley, A J; Catlow, C R A; Suwardiyanto; Collier, P; Hawkins, A P; Zachariou, Andrea; Lennon, David; Silverwood, I P; Parker, S F; Howe, R F.

In: Catalysis Science & Technology, Vol. 8, No. 13, 2018, p. 3304-3312.

Research output: Contribution to journalArticle

Matam, SK, O'Malley, AJ, Catlow, CRA, Suwardiyanto, Collier, P, Hawkins, AP, Zachariou, A, Lennon, D, Silverwood, IP, Parker, SF & Howe, RF 2018, 'The effects of MTG catalysis on methanol mobility in ZSM-5' Catalysis Science & Technology, vol. 8, no. 13, pp. 3304-3312. https://doi.org/10.1039/C8CY00422F
Matam SK, O'Malley AJ, Catlow CRA, Suwardiyanto, Collier P, Hawkins AP et al. The effects of MTG catalysis on methanol mobility in ZSM-5. Catalysis Science & Technology. 2018;8(13):3304-3312. https://doi.org/10.1039/C8CY00422F
Matam, S. K. ; O'Malley, A J ; Catlow, C R A ; Suwardiyanto ; Collier, P ; Hawkins, A P ; Zachariou, Andrea ; Lennon, David ; Silverwood, I P ; Parker, S F ; Howe, R F. / The effects of MTG catalysis on methanol mobility in ZSM-5. In: Catalysis Science & Technology. 2018 ; Vol. 8, No. 13. pp. 3304-3312.
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abstract = "We analyse the dynamics of methanol in ZSM-5 catalysts both with and without the hydrocarbon pool, resulting from the methanol to gasoline (MTG) reaction taking place at 623 K and 673 K for three days, to determine the effects of catalyst use on molecular mobility. Using quasielastic neutron scattering (QENS), we observe that methanol is immobile on the QENS instrumental time scale in the fresh catalyst (ZSM-5-F) and in the sample used to convert methanol for 3 days at 623 K (ZSM-5-623). However, in zeolite ZSM-5-673 (MTG at 673 K for 3 days) we observe isotropic methanol rotation with an immobile fraction of 0.58 and a rotational diffusion coefficient of DR = 3 × 1010 s−1. The observed differences between the zeolites in methanol dynamics are attributed to the development of mesoporosity in ZSM-5-673 due to the high reaction temperature of 673 K, leading to dislodgement of lattice Al as is evident from NMR data.",
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AU - Zachariou, Andrea

AU - Lennon, David

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N1 - The UK Catalysis Hub is thanked for resources and support provided via our membership of the UK Catalysis Hub Consortium and funded by EPSRC (grants EP/I038748/1, EP/I019693/1, EP/K014706/1, EP/K014668/1, EP/K014854/1, EP/ K014714/1 and EP/M013219/1). A. J. O. M. would like to acknowledge the Ramsay Trust for provision of the Ramsay Trust Memorial Fellowship. The STFC Rutherford Appleton Laboratory is thanked for access to neutron beam facilities.

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N2 - We analyse the dynamics of methanol in ZSM-5 catalysts both with and without the hydrocarbon pool, resulting from the methanol to gasoline (MTG) reaction taking place at 623 K and 673 K for three days, to determine the effects of catalyst use on molecular mobility. Using quasielastic neutron scattering (QENS), we observe that methanol is immobile on the QENS instrumental time scale in the fresh catalyst (ZSM-5-F) and in the sample used to convert methanol for 3 days at 623 K (ZSM-5-623). However, in zeolite ZSM-5-673 (MTG at 673 K for 3 days) we observe isotropic methanol rotation with an immobile fraction of 0.58 and a rotational diffusion coefficient of DR = 3 × 1010 s−1. The observed differences between the zeolites in methanol dynamics are attributed to the development of mesoporosity in ZSM-5-673 due to the high reaction temperature of 673 K, leading to dislodgement of lattice Al as is evident from NMR data.

AB - We analyse the dynamics of methanol in ZSM-5 catalysts both with and without the hydrocarbon pool, resulting from the methanol to gasoline (MTG) reaction taking place at 623 K and 673 K for three days, to determine the effects of catalyst use on molecular mobility. Using quasielastic neutron scattering (QENS), we observe that methanol is immobile on the QENS instrumental time scale in the fresh catalyst (ZSM-5-F) and in the sample used to convert methanol for 3 days at 623 K (ZSM-5-623). However, in zeolite ZSM-5-673 (MTG at 673 K for 3 days) we observe isotropic methanol rotation with an immobile fraction of 0.58 and a rotational diffusion coefficient of DR = 3 × 1010 s−1. The observed differences between the zeolites in methanol dynamics are attributed to the development of mesoporosity in ZSM-5-673 due to the high reaction temperature of 673 K, leading to dislodgement of lattice Al as is evident from NMR data.

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