Effects of crystal size on methanol to hydrocarbon conversion over single crystals of ZSM-5 studied by synchrotron infrared microspectroscopy

Ivalina B. Minova; Santhosh K. Matam; Alex Greenaway; C. Richard A. Catlow; Mark D. Frogley; Gianfelice Cinque; Paul A. Wright; Russell F. Howe

doi:10.1039/d0cp00704h

Effects of crystal size on methanol to hydrocarbon conversion over single crystals of ZSM-5 studied by synchrotron infrared microspectroscopy

Ivalina B. Minova, Santhosh K. Matam, Alex Greenaway, C. Richard A. Catlow, Mark D. Frogley, Gianfelice Cinque, Paul A. Wright, Russell F. Howe

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

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Abstract

Operando synchrotron infrared microspectroscopy (OIMS) was used to study the conversion of methanol over coffin-shaped HZSM-5 crystals of different sizes: large (∼250 × 80 × 85 μm³), medium (∼160 × 60 × 60 μm³) and small (∼55 × 30 × 30 μm³). The induction period, for direct alkene formation by deprotonation of surface methoxy groups, was found to decrease with decreasing crystal size and with increasing reaction temperature. Experiments with a continuous flow of dimethylether showed that evolution of the hydrocarbon pool and indirect alkene formation is also strongly dependent on crystal size. These measurements suggest that the hydrocarbon pool formation and indirect alkene generation should be almost instantaneous at reaction temperatures used in practical catalysis with crystal sizes typically ∼1 μm³.

Original language	English
Pages (from-to)	18849-18859
Number of pages	11
Journal	Physical chemistry chemical physics : PCCP
Volume	22
Issue number	34
Early online date	5 Mar 2020
DOIs	https://doi.org/10.1039/d0cp00704h
Publication status	Published - 14 Sept 2020

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10.1039/d0cp00704h

CRITICAT CDT: Critical Resource Catalysis - CRITICAT
Smith, A. D. (PI), Nolan, S. P. (CoI) & Westwood, N. J. (CoI)
EPSRC
1/05/14 → 31/10/22
Project: Standard

Effects of Crystal Size on Methanol to Hydrocarbon Conversion over Single Crystals of ZSM-5 Studied by Synchrotron Infrared Microspectroscopy (dataset)
Minova, I. (Creator), Matam, S. (Creator), Greenaway, A. (Creator), Catlow, R. (Creator), Frogley, M. (Creator), Cinque, G. (Creator), Wright, P. A. (Creator) & Howe, R. (Creator), University of St Andrews, 2020
DOI: 10.17630/306bd3c3-014b-466f-9538-b107628c847d
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title = "Effects of crystal size on methanol to hydrocarbon conversion over single crystals of ZSM-5 studied by synchrotron infrared microspectroscopy",

abstract = "Operando synchrotron infrared microspectroscopy (OIMS) was used to study the conversion of methanol over coffin-shaped HZSM-5 crystals of different sizes: large (∼250 × 80 × 85 μm3), medium (∼160 × 60 × 60 μm3) and small (∼55 × 30 × 30 μm3). The induction period, for direct alkene formation by deprotonation of surface methoxy groups, was found to decrease with decreasing crystal size and with increasing reaction temperature. Experiments with a continuous flow of dimethylether showed that evolution of the hydrocarbon pool and indirect alkene formation is also strongly dependent on crystal size. These measurements suggest that the hydrocarbon pool formation and indirect alkene generation should be almost instantaneous at reaction temperatures used in practical catalysis with crystal sizes typically ∼1 μm3.",

author = "Minova, {Ivalina B.} and Matam, {Santhosh K.} and Alex Greenaway and Catlow, {C. Richard A.} and Frogley, {Mark D.} and Gianfelice Cinque and Wright, {Paul A.} and Howe, {Russell F.}",

note = "IBM and PAW would like to thank the EPSRC and CRITICAT Centre for Doctoral Training for Financial Support [PhD studentship to IBM, and supplementary equipment grant EP/L016419/1]. The UK Catalysis Hub is thanked for resources and support provided via 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). We thank the Diamond Light Source for provision of beam time and support facilities at the MIRIAM beamline B22 (Experiments SM13725-1, SM16257-1, SM18680-1, SM20906-1). The research data supporting this publication can be accessed at https://doi.org/10.17630/306bd3c3-014b-466f-9538-b107628c847d.",

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AU - Minova, Ivalina B.

AU - Matam, Santhosh K.

AU - Greenaway, Alex

AU - Catlow, C. Richard A.

AU - Frogley, Mark D.

AU - Cinque, Gianfelice

AU - Wright, Paul A.

AU - Howe, Russell F.

N1 - IBM and PAW would like to thank the EPSRC and CRITICAT Centre for Doctoral Training for Financial Support [PhD studentship to IBM, and supplementary equipment grant EP/L016419/1]. The UK Catalysis Hub is thanked for resources and support provided via 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). We thank the Diamond Light Source for provision of beam time and support facilities at the MIRIAM beamline B22 (Experiments SM13725-1, SM16257-1, SM18680-1, SM20906-1). The research data supporting this publication can be accessed at https://doi.org/10.17630/306bd3c3-014b-466f-9538-b107628c847d.

PY - 2020/9/14

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N2 - Operando synchrotron infrared microspectroscopy (OIMS) was used to study the conversion of methanol over coffin-shaped HZSM-5 crystals of different sizes: large (∼250 × 80 × 85 μm3), medium (∼160 × 60 × 60 μm3) and small (∼55 × 30 × 30 μm3). The induction period, for direct alkene formation by deprotonation of surface methoxy groups, was found to decrease with decreasing crystal size and with increasing reaction temperature. Experiments with a continuous flow of dimethylether showed that evolution of the hydrocarbon pool and indirect alkene formation is also strongly dependent on crystal size. These measurements suggest that the hydrocarbon pool formation and indirect alkene generation should be almost instantaneous at reaction temperatures used in practical catalysis with crystal sizes typically ∼1 μm3.

AB - Operando synchrotron infrared microspectroscopy (OIMS) was used to study the conversion of methanol over coffin-shaped HZSM-5 crystals of different sizes: large (∼250 × 80 × 85 μm3), medium (∼160 × 60 × 60 μm3) and small (∼55 × 30 × 30 μm3). The induction period, for direct alkene formation by deprotonation of surface methoxy groups, was found to decrease with decreasing crystal size and with increasing reaction temperature. Experiments with a continuous flow of dimethylether showed that evolution of the hydrocarbon pool and indirect alkene formation is also strongly dependent on crystal size. These measurements suggest that the hydrocarbon pool formation and indirect alkene generation should be almost instantaneous at reaction temperatures used in practical catalysis with crystal sizes typically ∼1 μm3.

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JO - Physical chemistry chemical physics : PCCP

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Effects of crystal size on methanol to hydrocarbon conversion over single crystals of ZSM-5 studied by synchrotron infrared microspectroscopy

Abstract

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Effects of Crystal Size on Methanol to Hydrocarbon Conversion over Single Crystals of ZSM-5 Studied by Synchrotron Infrared Microspectroscopy (dataset)

Cite this