Coaromatization of methane and propane over Ga supported on HZSM-5 catalysts: The effect of mesoporosity on deactivation behavior

Min Yeong Gim; Yong Hyun Lim; Kwan Young Lee; Do Heui Kim

doi:10.1016/j.fuel.2021.121497

Coaromatization of methane and propane over Ga supported on HZSM-5 catalysts: The effect of mesoporosity on deactivation behavior

Min Yeong Gim, Yong Hyun Lim, Kwan Young Lee, Do Heui Kim

Department of Chemical and Biological Engineering

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

Abstract

Ga supported on mesoporous HZSM-5 (GaO_y/meso-HZSM-5) and conventional HZSM-5 (GaO_y/micro-HZSM-5) catalysts were compared to investigate the effect of mesoporosity on the deactivation behavior in the coaromatization of methane and propane. The trend of reaction intermediate distribution between the catalysts became gradually different with time-on-stream, implying a distinction in deactivation behavior. These are attributed to the behavior of acid site blockage, because the production of BTX are driven by acid sites. The reaction with ¹³CH₄ and further analyses revealed that the interaction between coke and Ga species that serve as Lewis acid sites is much stronger in GaO_y/micro-HZSM-5 than in GaO_y/meso-HZSM-5 post-reaction catalyst. Therefore, large amount of highly condensed coke was deposited in GaO_y/micro-HZSM-5 during the reaction, leading to fast catalyst deactivation. Consequently, the structural difference arising from mesoporosity affects physicochemical properties of the catalysts thereby contributing to different deactivation behavior between the catalysts.

Original language	English
Article number	121497
Journal	Fuel
Volume	304
DOIs	https://doi.org/10.1016/j.fuel.2021.121497
Publication status	Published - 2021 Nov 15

Keywords

Acid site blockage
Coaromatization of methane and propane
Coke analysis
Deactivation behavior
Ga supported on HZSM-5

ASJC Scopus subject areas

Chemical Engineering(all)
Fuel Technology
Energy Engineering and Power Technology
Organic Chemistry

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10.1016/j.fuel.2021.121497

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title = "Coaromatization of methane and propane over Ga supported on HZSM-5 catalysts: The effect of mesoporosity on deactivation behavior",

abstract = "Ga supported on mesoporous HZSM-5 (GaOy/meso-HZSM-5) and conventional HZSM-5 (GaOy/micro-HZSM-5) catalysts were compared to investigate the effect of mesoporosity on the deactivation behavior in the coaromatization of methane and propane. The trend of reaction intermediate distribution between the catalysts became gradually different with time-on-stream, implying a distinction in deactivation behavior. These are attributed to the behavior of acid site blockage, because the production of BTX are driven by acid sites. The reaction with 13CH4 and further analyses revealed that the interaction between coke and Ga species that serve as Lewis acid sites is much stronger in GaOy/micro-HZSM-5 than in GaOy/meso-HZSM-5 post-reaction catalyst. Therefore, large amount of highly condensed coke was deposited in GaOy/micro-HZSM-5 during the reaction, leading to fast catalyst deactivation. Consequently, the structural difference arising from mesoporosity affects physicochemical properties of the catalysts thereby contributing to different deactivation behavior between the catalysts.",

keywords = "Acid site blockage, Coaromatization of methane and propane, Coke analysis, Deactivation behavior, Ga supported on HZSM-5",

author = "{Yeong Gim}, Min and {Hyun Lim}, Yong and Lee, {Kwan Young} and {Heui Kim}, Do",

note = "Funding Information: This research was supported by C1 Gas Refinery Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT ( 2021M3D3A1A01022109 ). The Institute of Engineering Research at Seoul National University partially supported the research facilities for this work. Publisher Copyright: {\textcopyright} 2021 Elsevier Ltd",

year = "2021",

month = nov,

day = "15",

doi = "10.1016/j.fuel.2021.121497",

language = "English",

volume = "304",

journal = "Fuel",

issn = "0016-2361",

publisher = "Elsevier BV",

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TY - JOUR

T1 - Coaromatization of methane and propane over Ga supported on HZSM-5 catalysts

T2 - The effect of mesoporosity on deactivation behavior

AU - Yeong Gim, Min

AU - Hyun Lim, Yong

AU - Lee, Kwan Young

AU - Heui Kim, Do

N1 - Funding Information: This research was supported by C1 Gas Refinery Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT ( 2021M3D3A1A01022109 ). The Institute of Engineering Research at Seoul National University partially supported the research facilities for this work. Publisher Copyright: © 2021 Elsevier Ltd

PY - 2021/11/15

Y1 - 2021/11/15

N2 - Ga supported on mesoporous HZSM-5 (GaOy/meso-HZSM-5) and conventional HZSM-5 (GaOy/micro-HZSM-5) catalysts were compared to investigate the effect of mesoporosity on the deactivation behavior in the coaromatization of methane and propane. The trend of reaction intermediate distribution between the catalysts became gradually different with time-on-stream, implying a distinction in deactivation behavior. These are attributed to the behavior of acid site blockage, because the production of BTX are driven by acid sites. The reaction with 13CH4 and further analyses revealed that the interaction between coke and Ga species that serve as Lewis acid sites is much stronger in GaOy/micro-HZSM-5 than in GaOy/meso-HZSM-5 post-reaction catalyst. Therefore, large amount of highly condensed coke was deposited in GaOy/micro-HZSM-5 during the reaction, leading to fast catalyst deactivation. Consequently, the structural difference arising from mesoporosity affects physicochemical properties of the catalysts thereby contributing to different deactivation behavior between the catalysts.

AB - Ga supported on mesoporous HZSM-5 (GaOy/meso-HZSM-5) and conventional HZSM-5 (GaOy/micro-HZSM-5) catalysts were compared to investigate the effect of mesoporosity on the deactivation behavior in the coaromatization of methane and propane. The trend of reaction intermediate distribution between the catalysts became gradually different with time-on-stream, implying a distinction in deactivation behavior. These are attributed to the behavior of acid site blockage, because the production of BTX are driven by acid sites. The reaction with 13CH4 and further analyses revealed that the interaction between coke and Ga species that serve as Lewis acid sites is much stronger in GaOy/micro-HZSM-5 than in GaOy/meso-HZSM-5 post-reaction catalyst. Therefore, large amount of highly condensed coke was deposited in GaOy/micro-HZSM-5 during the reaction, leading to fast catalyst deactivation. Consequently, the structural difference arising from mesoporosity affects physicochemical properties of the catalysts thereby contributing to different deactivation behavior between the catalysts.

KW - Acid site blockage

KW - Coaromatization of methane and propane

KW - Coke analysis

KW - Deactivation behavior

KW - Ga supported on HZSM-5

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Coaromatization of methane and propane over Ga supported on HZSM-5 catalysts: The effect of mesoporosity on deactivation behavior

Abstract

Keywords

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