Methanol diffusion in H-ZSM-5 catalysts as a function of loading and Si/Al ratio: A classical molecular dynamics study

Claire Louise M. Woodward; Alexander J. Porter; Katie S.C. Morton; Alexander J. O'Malley

doi:10.1016/j.catcom.2022.106415

Methanol diffusion in H-ZSM-5 catalysts as a function of loading and Si/Al ratio: A classical molecular dynamics study

Claire Louise M. Woodward, Alexander J. Porter, Katie S.C. Morton, Alexander J. O'Malley

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

8 Citations (SciVal)

Abstract

Methanol diffusion in H-ZSM-5 was studied using classical molecular dynamics at 373 –423 K, using loadings of 3 and 5 molecules per unit cell, in frameworks with Si/Al = 15, 47, 95 191 and a fully siliceous system. While the lower loading exhibits higher diffusivity, self-diffusivities increase at both loadings between Si/Al = 15 and 95, after which they are independent of composition. The trend in diffusivity with Si/Al ratio is explained in terms of methanol-acid site interactions, while the trend with loading is explained in terms of methanol-methanol interactions and the resulting methanol structure in the catalyst pores.

Original language	English
Article number	106415
Journal	Catalysis Communications
Volume	164
Early online date	31 Jan 2022
DOIs	https://doi.org/10.1016/j.catcom.2022.106415
Publication status	Published - 30 Apr 2022

Bibliographical note

Funding Information:
CLMW acknowledges IChemE for the funding and the provision of the Syd Andrew Studentship. KSCM acknowledges the ISIS Neutron and Muon source for provision of an ISIS facilities development studentship and the UK Engineering and Physical Sciences Research Council (EPSRC) grant EP/T518013/1 for the University of Bath. AJP acknowledges the UK Engineering and Physical Sciences Research Council (EPSRC) grant EP/R513155/1 for the University of Bath. AJOM acknowledges Roger and Sue Whorrod for the funding of a Whorrod Fellowship. This research made use of the Balena High Performance Computing (HPC) Service at the University of Bath.

Keywords

Methanol-to-hydrocarbons
Molecular dynamics
Zeolites
ZSM-5

ASJC Scopus subject areas

Catalysis
General Chemistry
Process Chemistry and Technology

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10.1016/j.catcom.2022.106415Licence: CC BY

Cite this

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title = "Methanol diffusion in H-ZSM-5 catalysts as a function of loading and Si/Al ratio: A classical molecular dynamics study",

abstract = "Methanol diffusion in H-ZSM-5 was studied using classical molecular dynamics at 373 –423 K, using loadings of 3 and 5 molecules per unit cell, in frameworks with Si/Al = 15, 47, 95 191 and a fully siliceous system. While the lower loading exhibits higher diffusivity, self-diffusivities increase at both loadings between Si/Al = 15 and 95, after which they are independent of composition. The trend in diffusivity with Si/Al ratio is explained in terms of methanol-acid site interactions, while the trend with loading is explained in terms of methanol-methanol interactions and the resulting methanol structure in the catalyst pores.",

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author = "Woodward, {Claire Louise M.} and Porter, {Alexander J.} and Morton, {Katie S.C.} and O'Malley, {Alexander J.}",

note = "Funding Information: CLMW acknowledges IChemE for the funding and the provision of the Syd Andrew Studentship. KSCM acknowledges the ISIS Neutron and Muon source for provision of an ISIS facilities development studentship and the UK Engineering and Physical Sciences Research Council (EPSRC) grant EP/T518013/1 for the University of Bath. AJP acknowledges the UK Engineering and Physical Sciences Research Council (EPSRC) grant EP/R513155/1 for the University of Bath. AJOM acknowledges Roger and Sue Whorrod for the funding of a Whorrod Fellowship. This research made use of the Balena High Performance Computing (HPC) Service at the University of Bath. ",

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doi = "10.1016/j.catcom.2022.106415",

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AU - Woodward, Claire Louise M.

AU - Porter, Alexander J.

AU - Morton, Katie S.C.

AU - O'Malley, Alexander J.

N1 - Funding Information: CLMW acknowledges IChemE for the funding and the provision of the Syd Andrew Studentship. KSCM acknowledges the ISIS Neutron and Muon source for provision of an ISIS facilities development studentship and the UK Engineering and Physical Sciences Research Council (EPSRC) grant EP/T518013/1 for the University of Bath. AJP acknowledges the UK Engineering and Physical Sciences Research Council (EPSRC) grant EP/R513155/1 for the University of Bath. AJOM acknowledges Roger and Sue Whorrod for the funding of a Whorrod Fellowship. This research made use of the Balena High Performance Computing (HPC) Service at the University of Bath.

PY - 2022/4/30

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N2 - Methanol diffusion in H-ZSM-5 was studied using classical molecular dynamics at 373 –423 K, using loadings of 3 and 5 molecules per unit cell, in frameworks with Si/Al = 15, 47, 95 191 and a fully siliceous system. While the lower loading exhibits higher diffusivity, self-diffusivities increase at both loadings between Si/Al = 15 and 95, after which they are independent of composition. The trend in diffusivity with Si/Al ratio is explained in terms of methanol-acid site interactions, while the trend with loading is explained in terms of methanol-methanol interactions and the resulting methanol structure in the catalyst pores.

AB - Methanol diffusion in H-ZSM-5 was studied using classical molecular dynamics at 373 –423 K, using loadings of 3 and 5 molecules per unit cell, in frameworks with Si/Al = 15, 47, 95 191 and a fully siliceous system. While the lower loading exhibits higher diffusivity, self-diffusivities increase at both loadings between Si/Al = 15 and 95, after which they are independent of composition. The trend in diffusivity with Si/Al ratio is explained in terms of methanol-acid site interactions, while the trend with loading is explained in terms of methanol-methanol interactions and the resulting methanol structure in the catalyst pores.

KW - Methanol-to-hydrocarbons

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KW - Zeolites

KW - ZSM-5

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Methanol diffusion in H-ZSM-5 catalysts as a function of loading and Si/Al ratio: A classical molecular dynamics study

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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