Non-oxidative aromatization and ethylene formation over Ga/HZSM-5 catalysts using a mixed feed of methane and ethane

Byung Jin Lee; Young Gul Hur; Do Huei Kim; Seong Ho Lee; Kwan Young Lee

doi:10.1016/j.fuel.2019.05.014

Non-oxidative aromatization and ethylene formation over Ga/HZSM-5 catalysts using a mixed feed of methane and ethane

Byung Jin Lee, Young Gul Hur, Do Huei Kim, Seong Ho Lee, Kwan Young Lee

Department of Chemical and Biological Engineering

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

35 Citations (Scopus)

Abstract

The effects of the total number of acid site and gallium loading on Ga/HZSM-5 catalysts for non-oxidative aromatization and ethylene formation were investigated using a mixed feed of methane and ethane, analogous to shale gas. When the acid sites of the catalysts increased with the change in the Si/Al ratio, the total conversion of hydrocarbons and the total yield of BTX and ethylene increased, but the selectivity of ethylene tended to decrease. This suggests that the Brønsted acid sites of catalysts is responsible for the dispersion of gallium species and the aromatization of intermediate. On the other hand, when the gallium loading of HZSM-5(15)catalysts increased from 1.0 to 7.0 wt%, the ethylene yield increased, but the BTX yield decreased. The excessive gallium loading resulted in the drastic change of textural properties and the dealumination leading to the decrease of Brønsted acid sites, which caused the decrease of BTX selectivity and the increase of ethylene selectivity. In addition, with the increase of the gallium loading of the HZSM-5(15)catalysts, while the ethane conversion did not change, the methane conversion and ethylene yield gradually increased. This suggests that the dehydrogenative coupling of methane was promoted by the gallium species formed at high gallium loading catalysts such as gallyl ion. Characterizations by N₂ adsorption/desorption, ICP-AES, XRD, XPS, TEM, NH₃-TPD, pyridine FT-IR, H₂-TPR, AAS, and ²⁷Al NMR were used to investigate the relationship between the catalytic performance for aromatization and ethylene formation.

Original language	English
Pages (from-to)	449-459
Number of pages	11
Journal	Fuel
Volume	253
DOIs	https://doi.org/10.1016/j.fuel.2019.05.014
Publication status	Published - 2019 Oct 1

Bibliographical note

Funding Information:
We thank Elizabeth Bickel for technical feedback on this manuscript. This research was supported by the C1 Gas Refinery Program through the National Research Foundation of Korea (NRF)and funded by the Ministry of Science, ICT & Future Planning (2016M3D3A1A01913252). Also, this work was supported by a National Research Foundation of Korea (NRF)grant funded by the Korean Government (MSIP)(NRF-2015R1A2A1A13001856).

Keywords

BTX
Dehydrogenative coupling of methane
Ethylene
Ga/HZSM-5
Non-oxidative aromatization
Shale gas

ASJC Scopus subject areas

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

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10.1016/j.fuel.2019.05.014

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@article{d8dc24d541d044c68ecc35bcc3b4d4ff,

title = "Non-oxidative aromatization and ethylene formation over Ga/HZSM-5 catalysts using a mixed feed of methane and ethane",

abstract = "The effects of the total number of acid site and gallium loading on Ga/HZSM-5 catalysts for non-oxidative aromatization and ethylene formation were investigated using a mixed feed of methane and ethane, analogous to shale gas. When the acid sites of the catalysts increased with the change in the Si/Al ratio, the total conversion of hydrocarbons and the total yield of BTX and ethylene increased, but the selectivity of ethylene tended to decrease. This suggests that the Br{\o}nsted acid sites of catalysts is responsible for the dispersion of gallium species and the aromatization of intermediate. On the other hand, when the gallium loading of HZSM-5(15)catalysts increased from 1.0 to 7.0 wt%, the ethylene yield increased, but the BTX yield decreased. The excessive gallium loading resulted in the drastic change of textural properties and the dealumination leading to the decrease of Br{\o}nsted acid sites, which caused the decrease of BTX selectivity and the increase of ethylene selectivity. In addition, with the increase of the gallium loading of the HZSM-5(15)catalysts, while the ethane conversion did not change, the methane conversion and ethylene yield gradually increased. This suggests that the dehydrogenative coupling of methane was promoted by the gallium species formed at high gallium loading catalysts such as gallyl ion. Characterizations by N2 adsorption/desorption, ICP-AES, XRD, XPS, TEM, NH3-TPD, pyridine FT-IR, H2-TPR, AAS, and 27Al NMR were used to investigate the relationship between the catalytic performance for aromatization and ethylene formation.",

keywords = "BTX, Dehydrogenative coupling of methane, Ethylene, Ga/HZSM-5, Non-oxidative aromatization, Shale gas",

author = "Lee, {Byung Jin} and Hur, {Young Gul} and Kim, {Do Huei} and Lee, {Seong Ho} and Lee, {Kwan Young}",

note = "Funding Information: We thank Elizabeth Bickel for technical feedback on this manuscript. This research was supported by the C1 Gas Refinery Program through the National Research Foundation of Korea (NRF)and funded by the Ministry of Science, ICT & Future Planning (2016M3D3A1A01913252). Also, this work was supported by a National Research Foundation of Korea (NRF)grant funded by the Korean Government (MSIP)(NRF-2015R1A2A1A13001856).",

year = "2019",

month = oct,

day = "1",

doi = "10.1016/j.fuel.2019.05.014",

language = "English",

volume = "253",

pages = "449--459",

journal = "Fuel",

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TY - JOUR

T1 - Non-oxidative aromatization and ethylene formation over Ga/HZSM-5 catalysts using a mixed feed of methane and ethane

AU - Lee, Byung Jin

AU - Hur, Young Gul

AU - Kim, Do Huei

AU - Lee, Seong Ho

AU - Lee, Kwan Young

N1 - Funding Information: We thank Elizabeth Bickel for technical feedback on this manuscript. This research was supported by the C1 Gas Refinery Program through the National Research Foundation of Korea (NRF)and funded by the Ministry of Science, ICT & Future Planning (2016M3D3A1A01913252). Also, this work was supported by a National Research Foundation of Korea (NRF)grant funded by the Korean Government (MSIP)(NRF-2015R1A2A1A13001856).

PY - 2019/10/1

Y1 - 2019/10/1

N2 - The effects of the total number of acid site and gallium loading on Ga/HZSM-5 catalysts for non-oxidative aromatization and ethylene formation were investigated using a mixed feed of methane and ethane, analogous to shale gas. When the acid sites of the catalysts increased with the change in the Si/Al ratio, the total conversion of hydrocarbons and the total yield of BTX and ethylene increased, but the selectivity of ethylene tended to decrease. This suggests that the Brønsted acid sites of catalysts is responsible for the dispersion of gallium species and the aromatization of intermediate. On the other hand, when the gallium loading of HZSM-5(15)catalysts increased from 1.0 to 7.0 wt%, the ethylene yield increased, but the BTX yield decreased. The excessive gallium loading resulted in the drastic change of textural properties and the dealumination leading to the decrease of Brønsted acid sites, which caused the decrease of BTX selectivity and the increase of ethylene selectivity. In addition, with the increase of the gallium loading of the HZSM-5(15)catalysts, while the ethane conversion did not change, the methane conversion and ethylene yield gradually increased. This suggests that the dehydrogenative coupling of methane was promoted by the gallium species formed at high gallium loading catalysts such as gallyl ion. Characterizations by N2 adsorption/desorption, ICP-AES, XRD, XPS, TEM, NH3-TPD, pyridine FT-IR, H2-TPR, AAS, and 27Al NMR were used to investigate the relationship between the catalytic performance for aromatization and ethylene formation.

AB - The effects of the total number of acid site and gallium loading on Ga/HZSM-5 catalysts for non-oxidative aromatization and ethylene formation were investigated using a mixed feed of methane and ethane, analogous to shale gas. When the acid sites of the catalysts increased with the change in the Si/Al ratio, the total conversion of hydrocarbons and the total yield of BTX and ethylene increased, but the selectivity of ethylene tended to decrease. This suggests that the Brønsted acid sites of catalysts is responsible for the dispersion of gallium species and the aromatization of intermediate. On the other hand, when the gallium loading of HZSM-5(15)catalysts increased from 1.0 to 7.0 wt%, the ethylene yield increased, but the BTX yield decreased. The excessive gallium loading resulted in the drastic change of textural properties and the dealumination leading to the decrease of Brønsted acid sites, which caused the decrease of BTX selectivity and the increase of ethylene selectivity. In addition, with the increase of the gallium loading of the HZSM-5(15)catalysts, while the ethane conversion did not change, the methane conversion and ethylene yield gradually increased. This suggests that the dehydrogenative coupling of methane was promoted by the gallium species formed at high gallium loading catalysts such as gallyl ion. Characterizations by N2 adsorption/desorption, ICP-AES, XRD, XPS, TEM, NH3-TPD, pyridine FT-IR, H2-TPR, AAS, and 27Al NMR were used to investigate the relationship between the catalytic performance for aromatization and ethylene formation.

KW - BTX

KW - Dehydrogenative coupling of methane

KW - Ethylene

KW - Ga/HZSM-5

KW - Non-oxidative aromatization

KW - Shale gas

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U2 - 10.1016/j.fuel.2019.05.014

DO - 10.1016/j.fuel.2019.05.014

M3 - Article

AN - SCOPUS:85065520562

SN - 0016-2361

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EP - 459

JO - Fuel

JF - Fuel

ER -

Non-oxidative aromatization and ethylene formation over Ga/HZSM-5 catalysts using a mixed feed of methane and ethane

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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