Elementary steps in the formation of hydrocarbons from surface methoxy groups in HZSM-5 seen by synchrotron infrared microspectroscopy

Ivalina Minova; Santhosh Matam; Alex Greenaway; Richard Catlow; Mark Frogley; Gianfelice Cinque; Paul A. Wright; Russell Howe

doi:10.1021/acscatal.9b01820

Elementary steps in the formation of hydrocarbons from surface methoxy groups in HZSM-5 seen by synchrotron infrared microspectroscopy

Ivalina Minova, Santhosh Matam, Alex Greenaway, Richard Catlow, Mark Frogley, Gianfelice Cinque, Paul A. Wright, Russell Howe

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

Abstract

Synchrotron infrared microspectroscopy has identified with high temporal resolution (down to 0.25 s) the initial events occurring when methanol vapor is in contact with a crystal of zeolite HZSM-5. The first alkenes are generated directly from methoxy groups formed at the acid sites via their deprotonation. These alkenes can either desorb directly or oligomerize and cyclize to form dimethylcyclopentenyl cations. The oligomeric and dimethylcyclopentenyl cations are the first major components of the hydrocarbon pool that precede aromatic hydrocarbons and lead to indirect alkene formation. The technique observes these events in real time.

Original language	English
Pages (from-to)	6564-6570
Number of pages	7
Journal	ACS Catalysis
Volume	9
Early online date	17 Jun 2019
DOIs	https://doi.org/10.1021/acscatal.9b01820
Publication status	E-pub ahead of print - 17 Jun 2019

Keywords

Synchrotron infrared microspectroscopy
ZSM-5
Methanol-to-hydrocarbons
Hydrocarbon pool
Carbon-carbon bond formation
Micro-FTIR

Access to Document

10.1021/acscatal.9b01820

Main Text_Final MS file
Copyright © 2019 American Chemical Society. This work has been made available online in accordance with the publisher’s policies. This is the author created, accepted version manuscript following peer review and may differ slightly from the final published version. The final published version of this work is available at https://doi.org/10.1021/acscatal.9b01820
Accepted author manuscript, 572 KB
Sup Info_SI Final versionAccepted author manuscript, 935 KB

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

Elementary Steps in the Formation of Hydrocarbons from Surface Methoxy Groups in HZSM-5 seen by Synchrotron Infrared Microspectroscopy (dataset)
Minova, I. (Creator), Matam, S. K. (Creator), Greenaway, A. (Creator), Catlow, R. A. (Creator), Frogley, M. D. (Creator), Cinque, G. (Creator), Wright, P. A. (Creator) & Howe, R. F. (Creator), University of St Andrews, 19 Jul 2019
DOI: 10.17630/d0e5a924-8850-4fe4-a56f-b00c7472f25a
Dataset

File

Cite this

@article{33cde3ead487475b821677438d27dff5,

title = "Elementary steps in the formation of hydrocarbons from surface methoxy groups in HZSM-5 seen by synchrotron infrared microspectroscopy",

abstract = "Synchrotron infrared microspectroscopy has identified with high temporal resolution (down to 0.25 s) the initial events occurring when methanol vapor is in contact with a crystal of zeolite HZSM-5. The first alkenes are generated directly from methoxy groups formed at the acid sites via their deprotonation. These alkenes can either desorb directly or oligomerize and cyclize to form dimethylcyclopentenyl cations. The oligomeric and dimethylcyclopentenyl cations are the first major components of the hydrocarbon pool that precede aromatic hydrocarbons and lead to indirect alkene formation. The technique observes these events in real time.",

keywords = "Synchrotron infrared microspectroscopy, ZSM-5, Methanol-to-hydrocarbons, Hydrocarbon pool, Carbon-carbon bond formation, Micro-FTIR",

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

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).",

year = "2019",

month = jun,

day = "17",

doi = "10.1021/acscatal.9b01820",

language = "English",

volume = "9",

pages = "6564--6570",

journal = "ACS Catalysis",

issn = "2155-5435",

publisher = "American Chemical Society (ACS)",

}

TY - JOUR

T1 - Elementary steps in the formation of hydrocarbons from surface methoxy groups in HZSM-5 seen by synchrotron infrared microspectroscopy

AU - Minova, Ivalina

AU - Matam, Santhosh

AU - Greenaway, Alex

AU - Catlow, Richard

AU - Frogley, Mark

AU - Cinque, Gianfelice

AU - Wright, Paul A.

AU - Howe, Russell

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).

PY - 2019/6/17

Y1 - 2019/6/17

N2 - Synchrotron infrared microspectroscopy has identified with high temporal resolution (down to 0.25 s) the initial events occurring when methanol vapor is in contact with a crystal of zeolite HZSM-5. The first alkenes are generated directly from methoxy groups formed at the acid sites via their deprotonation. These alkenes can either desorb directly or oligomerize and cyclize to form dimethylcyclopentenyl cations. The oligomeric and dimethylcyclopentenyl cations are the first major components of the hydrocarbon pool that precede aromatic hydrocarbons and lead to indirect alkene formation. The technique observes these events in real time.

AB - Synchrotron infrared microspectroscopy has identified with high temporal resolution (down to 0.25 s) the initial events occurring when methanol vapor is in contact with a crystal of zeolite HZSM-5. The first alkenes are generated directly from methoxy groups formed at the acid sites via their deprotonation. These alkenes can either desorb directly or oligomerize and cyclize to form dimethylcyclopentenyl cations. The oligomeric and dimethylcyclopentenyl cations are the first major components of the hydrocarbon pool that precede aromatic hydrocarbons and lead to indirect alkene formation. The technique observes these events in real time.

KW - Synchrotron infrared microspectroscopy

KW - ZSM-5

KW - Methanol-to-hydrocarbons

KW - Hydrocarbon pool

KW - Carbon-carbon bond formation

KW - Micro-FTIR

U2 - 10.1021/acscatal.9b01820

DO - 10.1021/acscatal.9b01820

M3 - Article

SN - 2155-5435

VL - 9

SP - 6564

EP - 6570

JO - ACS Catalysis

JF - ACS Catalysis

ER -

Elementary steps in the formation of hydrocarbons from surface methoxy groups in HZSM-5 seen by synchrotron infrared microspectroscopy

Abstract

Keywords

Access to Document

Fingerprint

Projects

CRITICAT CDT: Critical Resource Catalysis - CRITICAT

Datasets

Elementary Steps in the Formation of Hydrocarbons from Surface Methoxy Groups in HZSM-5 seen by Synchrotron Infrared Microspectroscopy (dataset)

Cite this