The Effect of Co-feeding Methyl Acetate on the H-ZSM5 Catalysed Methanol-to-Hydrocarbons Reaction

A. Zachariou; A. P. Hawkins; P. Collier; R. F. Howe; S. F. Parker; D. Lennon

doi:10.1007/s11244-020-01258-3

The Effect of Co-feeding Methyl Acetate on the H-ZSM5 Catalysed Methanol-to-Hydrocarbons Reaction

A. Zachariou, A. P. Hawkins, P. Collier, R. F. Howe, S. F. Parker, D. Lennon^* (Corresponding Author)

^*Corresponding author for this work

Chemistry

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

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Abstract

The reactivity of methanol and methyl acetate mixtures over a HZSM-5 catalyst is studied over a period of 6 h at 350 °C, with small molecular weight olefins and aromatic compounds observed as reaction products. Post-reaction analysis of the catalyst shows the coke content to increase with methyl acetate content. Vibrational spectra (DRIFTS and inelastic neutron scattering, INS) indicate the major hydrocarbon species present in the coked catalysts to be methylated aromatic molecules, with INS spectra indicating a greater degree of methylation in the catalysts used with higher methyl acetate content. The greater extent of deactivation at higher methyl acetate concentrations is tentatively attributed to a diminishment of water in the zeolite cavity, which would otherwise facilitate re-generation of the active sites.

Original language	English
Pages (from-to)	370-377
Number of pages	8
Journal	Topics in Catalysis
Volume	63
Issue number	3-4
Early online date	3 Apr 2020
DOIs	https://doi.org/10.1007/s11244-020-01258-3
Publication status	Published - 1 Jul 2020

Bibliographical note

Funding Information:
Johnson Matthey plc and the EPSRC are thanked for postgraduate student support (A.P.H., A.Z.) via the Industrial CASE scheme (EP/P510506/1). Johnson Matthey plc is additionally thanked for provision of the ZSM-5 catalyst. The Science and Technology Facilities Council is thanked for the provision of neutron beam time (RB1820116, https://doi.org/10.5286/isis.e.97999822 ). The resources and support provided by the UK Catalysis Hub via Membership of the UK Catalysis Hub Consortium and funded by EPSRC (Grants EP/K014706/1, EP/K014668/1, EP/ K014854/1, EP/K014714/1, and EP/M013219/1) are gratefully acknowledged.

Keywords

HZSM-5
Inelastic neutron scattering
Methanol-to-hydrocarbons reaction
Methyl acetate

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title = "The Effect of Co-feeding Methyl Acetate on the H-ZSM5 Catalysed Methanol-to-Hydrocarbons Reaction",

abstract = "The reactivity of methanol and methyl acetate mixtures over a HZSM-5 catalyst is studied over a period of 6 h at 350 °C, with small molecular weight olefins and aromatic compounds observed as reaction products. Post-reaction analysis of the catalyst shows the coke content to increase with methyl acetate content. Vibrational spectra (DRIFTS and inelastic neutron scattering, INS) indicate the major hydrocarbon species present in the coked catalysts to be methylated aromatic molecules, with INS spectra indicating a greater degree of methylation in the catalysts used with higher methyl acetate content. The greater extent of deactivation at higher methyl acetate concentrations is tentatively attributed to a diminishment of water in the zeolite cavity, which would otherwise facilitate re-generation of the active sites.",

keywords = "HZSM-5, Inelastic neutron scattering, Methanol-to-hydrocarbons reaction, Methyl acetate",

author = "A. Zachariou and Hawkins, {A. P.} and P. Collier and Howe, {R. F.} and Parker, {S. F.} and D. Lennon",

note = "Funding Information: Johnson Matthey plc and the EPSRC are thanked for postgraduate student support (A.P.H., A.Z.) via the Industrial CASE scheme (EP/P510506/1). Johnson Matthey plc is additionally thanked for provision of the ZSM-5 catalyst. The Science and Technology Facilities Council is thanked for the provision of neutron beam time (RB1820116, https://doi.org/10.5286/isis.e.97999822 ). The resources and support provided by the UK Catalysis Hub via Membership of the UK Catalysis Hub Consortium and funded by EPSRC (Grants EP/K014706/1, EP/K014668/1, EP/ K014854/1, EP/K014714/1, and EP/M013219/1) are gratefully acknowledged. ",

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AU - Howe, R. F.

AU - Parker, S. F.

AU - Lennon, D.

N1 - Funding Information: Johnson Matthey plc and the EPSRC are thanked for postgraduate student support (A.P.H., A.Z.) via the Industrial CASE scheme (EP/P510506/1). Johnson Matthey plc is additionally thanked for provision of the ZSM-5 catalyst. The Science and Technology Facilities Council is thanked for the provision of neutron beam time (RB1820116, https://doi.org/10.5286/isis.e.97999822 ). The resources and support provided by the UK Catalysis Hub via Membership of the UK Catalysis Hub Consortium and funded by EPSRC (Grants EP/K014706/1, EP/K014668/1, EP/ K014854/1, EP/K014714/1, and EP/M013219/1) are gratefully acknowledged.

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N2 - The reactivity of methanol and methyl acetate mixtures over a HZSM-5 catalyst is studied over a period of 6 h at 350 °C, with small molecular weight olefins and aromatic compounds observed as reaction products. Post-reaction analysis of the catalyst shows the coke content to increase with methyl acetate content. Vibrational spectra (DRIFTS and inelastic neutron scattering, INS) indicate the major hydrocarbon species present in the coked catalysts to be methylated aromatic molecules, with INS spectra indicating a greater degree of methylation in the catalysts used with higher methyl acetate content. The greater extent of deactivation at higher methyl acetate concentrations is tentatively attributed to a diminishment of water in the zeolite cavity, which would otherwise facilitate re-generation of the active sites.

AB - The reactivity of methanol and methyl acetate mixtures over a HZSM-5 catalyst is studied over a period of 6 h at 350 °C, with small molecular weight olefins and aromatic compounds observed as reaction products. Post-reaction analysis of the catalyst shows the coke content to increase with methyl acetate content. Vibrational spectra (DRIFTS and inelastic neutron scattering, INS) indicate the major hydrocarbon species present in the coked catalysts to be methylated aromatic molecules, with INS spectra indicating a greater degree of methylation in the catalysts used with higher methyl acetate content. The greater extent of deactivation at higher methyl acetate concentrations is tentatively attributed to a diminishment of water in the zeolite cavity, which would otherwise facilitate re-generation of the active sites.

KW - HZSM-5

KW - Inelastic neutron scattering

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The Effect of Co-feeding Methyl Acetate on the H-ZSM5 Catalysed Methanol-to-Hydrocarbons Reaction

Abstract

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Keywords

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