Elementary Steps in the Formation of Hydrocarbons from Surface Methoxy Groups in HZSM-5 Seen 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:10.1021/acscatal.9b01820

Elementary Steps in the Formation of Hydrocarbons from Surface Methoxy Groups in HZSM-5 Seen 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^* (Corresponding Author)

^*Corresponding author for this work

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

8 Citations (Scopus)

4 Downloads (Pure)

Abstract

Synchrotron infrared microspectroscopy has identified with high temporal resolution (down to 0.25 s) the initial events occurring when methanol vapour is contacted 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 oligomerise and cyclise 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
Issue number	7
Early online date	17 Jun 2019
DOIs	https://doi.org/10.1021/acscatal.9b01820
Publication status	Published - 5 Jul 2019

Keywords

synchrotron infrared microspectroscopy
ZSM-5
methanol-to-hydrocarbons
hydrocarbon pool
carbon-carbon bond formation
micro-FTIR

Access to Document

10.1021/acscatal.9b01820Licence: Unspecified

Accepted Manuscript
This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acscatal.9b01820.
Accepted author manuscript, 572 KBLicence: Unspecified
Accepted Supplementary InformationAccepted author manuscript, 935 KBLicence: Unspecified

Fingerprint Dive into the research topics of 'Elementary Steps in the Formation of Hydrocarbons from Surface Methoxy Groups in HZSM-5 Seen by Synchrotron Infrared Microspectroscopy'. Together they form a unique fingerprint.

Russell Howe
- Chemistry (Research Theme)
- School of Natural & Computing Sciences, Chemistry - Chair of Chemistry
Person: Academic

Cite this

Elementary Steps in the Formation of Hydrocarbons from Surface Methoxy Groups in HZSM-5 Seen by Synchrotron Infrared Microspectroscopy. / Minova, Ivalina B.; Matam, Santhosh K.; Greenaway, Alex; Catlow, C. Richard A. ; Frogley, Mark D.; Cinque, Gianfelice; Wright, Paul A.; Howe, Russell F. (Corresponding Author).

In: ACS Catalysis, Vol. 9, No. 7, 05.07.2019, p. 6564-6570.

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

@article{6f275d63987149a39c5c8006ecde4743,

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 vapour is contacted 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 oligomerise and cyclise 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 = "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).",

year = "2019",

month = jul,

day = "5",

doi = "10.1021/acscatal.9b01820",

language = "English",

volume = "9",

pages = "6564--6570",

journal = "ACS Catalysis",

issn = "2155-5435",

publisher = "AMER CHEMICAL SOC",

number = "7",

}

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 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).

PY - 2019/7/5

Y1 - 2019/7/5

N2 - Synchrotron infrared microspectroscopy has identified with high temporal resolution (down to 0.25 s) the initial events occurring when methanol vapour is contacted 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 oligomerise and cyclise 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 vapour is contacted 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 oligomerise and cyclise 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

UR - http://pubs.acs.org/doi/10.1021/acscatal.9b01820

UR - http://www.mendeley.com/research/elementary-steps-formation-hydrocarbons-surface-methoxy-groups-hzsm5-seen-synchrotron-infrared-micro

UR - http://www.scopus.com/inward/record.url?scp=85068414252&partnerID=8YFLogxK

U2 - 10.1021/acscatal.9b01820

DO - 10.1021/acscatal.9b01820

M3 - Article

VL - 9

SP - 6564

EP - 6570

JO - ACS Catalysis

JF - ACS Catalysis

SN - 2155-5435

IS - 7

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

Russell Howe

Cite this