PEPICO analysis of catalytic reactor effluents towards quantitative isomer discrimination : DME conversion over a ZSM-5 zeolite
Babayan, Morsal ; Redekop, Evgeniy ; Kokkonen, Esko LU
; Olsbye, Unni
; Huttula, Marko
and Urpelainen, Samuli
LU
(2024)
In Journal of Synchrotron Radiation
31(Pt 4).
p.841-850
- Abstract
The methanol-to-hydrocarbons (MTH) process involves the conversion of methanol, a C1 feedstock that can be produced from green sources, into hydrocarbons using shape-selective microporous acidic catalysts – zeolite and zeotypes. This reaction yields a complex mixture of species, some of which are highly reactive and/or present in several isomeric forms, posing significant challenges for effluent analysis. Conventional gas-phase chromatography (GC) is typically employed for the analysis of reaction products in laboratory flow reactors. However, GC is not suitable for the detection of highly reactive intermediates such as ketene or formaldehyde and is not suitable for kinetic studies under well defined low pressure conditions.... (More)
The methanol-to-hydrocarbons (MTH) process involves the conversion of methanol, a C1 feedstock that can be produced from green sources, into hydrocarbons using shape-selective microporous acidic catalysts – zeolite and zeotypes. This reaction yields a complex mixture of species, some of which are highly reactive and/or present in several isomeric forms, posing significant challenges for effluent analysis. Conventional gas-phase chromatography (GC) is typically employed for the analysis of reaction products in laboratory flow reactors. However, GC is not suitable for the detection of highly reactive intermediates such as ketene or formaldehyde and is not suitable for kinetic studies under well defined low pressure conditions. Photoelectron–photoion coincidence (PEPICO) spectroscopy has emerged as a powerful analytical tool for unraveling complex compositions of catalytic effluents, but its availability is limited to a handful of facilities worldwide. Herein, PEPICO analysis of catalytic reactor effluents has been implemented at the FinEstBeAMS beamline of MAX IV Laboratory. The conversion of dimethyl ether (DME) on a zeolite catalyst (ZSM-5-MFI27) is used as a prototypical model reaction producing a wide distribution of hydrocarbon products. Since in zeolites methanol is quickly equilibrated with DME, this reaction can be used to probe vast sub-networks of the full MTH process, while eliminating or at least slowing down methanol-induced secondary reactions and catalyst deactivation. Quantitative discrimination of xylene isomers in the effluent stream is achieved by deconvoluting the coincidence photoelectron spectra.
(Less)
- author
- Babayan, Morsal
; Redekop, Evgeniy
; Kokkonen, Esko
LU
; Olsbye, Unni
; Huttula, Marko
and Urpelainen, Samuli
LU
- organization
- publishing date
- 2024-07
- type
- Contribution to journal
- publication status
- published
- subject
- keywords
- dimethyl ether to hydrocarbons conversion, electron spectroscopy, ion mass spectrometry, isomer selectivity, PEPICO, reactor effluent analysis, synchrotron radiation, zeolite catalyst
- in
- Journal of Synchrotron Radiation
- volume
- 31
- issue
- Pt 4
- pages
- 10 pages
- publisher
- International Union of Crystallography
- external identifiers
-
- pmid:38917019
- scopus:85198525405
- ISSN
- 0909-0495
- DOI
- 10.1107/S1600577524004405
- language
- English
- LU publication?
- yes
- id
- 3abf70f2-4777-4763-8ece-2b953b66e799
- date added to LUP
- 2024-10-02 13:54:23
- date last changed
- 2025-06-12 12:17:47
@article{3abf70f2-4777-4763-8ece-2b953b66e799,
abstract = {{<p>The methanol-to-hydrocarbons (MTH) process involves the conversion of methanol, a C1 feedstock that can be produced from green sources, into hydrocarbons using shape-selective microporous acidic catalysts – zeolite and zeotypes. This reaction yields a complex mixture of species, some of which are highly reactive and/or present in several isomeric forms, posing significant challenges for effluent analysis. Conventional gas-phase chromatography (GC) is typically employed for the analysis of reaction products in laboratory flow reactors. However, GC is not suitable for the detection of highly reactive intermediates such as ketene or formaldehyde and is not suitable for kinetic studies under well defined low pressure conditions. Photoelectron–photoion coincidence (PEPICO) spectroscopy has emerged as a powerful analytical tool for unraveling complex compositions of catalytic effluents, but its availability is limited to a handful of facilities worldwide. Herein, PEPICO analysis of catalytic reactor effluents has been implemented at the FinEstBeAMS beamline of MAX IV Laboratory. The conversion of dimethyl ether (DME) on a zeolite catalyst (ZSM-5-MFI27) is used as a prototypical model reaction producing a wide distribution of hydrocarbon products. Since in zeolites methanol is quickly equilibrated with DME, this reaction can be used to probe vast sub-networks of the full MTH process, while eliminating or at least slowing down methanol-induced secondary reactions and catalyst deactivation. Quantitative discrimination of xylene isomers in the effluent stream is achieved by deconvoluting the coincidence photoelectron spectra.</p>}},
author = {{Babayan, Morsal and Redekop, Evgeniy and Kokkonen, Esko and Olsbye, Unni and Huttula, Marko and Urpelainen, Samuli}},
issn = {{0909-0495}},
keywords = {{dimethyl ether to hydrocarbons conversion; electron spectroscopy; ion mass spectrometry; isomer selectivity; PEPICO; reactor effluent analysis; synchrotron radiation; zeolite catalyst}},
language = {{eng}},
number = {{Pt 4}},
pages = {{841--850}},
publisher = {{International Union of Crystallography}},
series = {{Journal of Synchrotron Radiation}},
title = {{PEPICO analysis of catalytic reactor effluents towards quantitative isomer discrimination : DME conversion over a ZSM-5 zeolite}},
url = {{http://dx.doi.org/10.1107/S1600577524004405}},
doi = {{10.1107/S1600577524004405}},
volume = {{31}},
year = {{2024}},
}