Controllably tailoring external surface sites of nanosheet HZSM-5 for maximizing light olefins in catalytic cracking of n-decane

doi:10.1016/j.cjche.2021.04.015

中国化学工程学报 ›› 2021, Vol. 38 ›› Issue (10): 276-285.DOI: 10.1016/j.cjche.2021.04.015

• Materials and Product Engineering • 上一篇下一篇

Controllably tailoring external surface sites of nanosheet HZSM-5 for maximizing light olefins in catalytic cracking of n-decane

Tiantian Zhu¹, Hairui Liang¹, Bofeng Zhang¹, Yajie Tian², Guozhu Liu¹

1. Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
2. Henan Province Engineering Research Center of Catalytic Reaction, College of Chemistry and Chemical Engineering, Henan University, Kaifeng 475004, China

收稿日期:2021-02-10 修回日期:2021-04-04 出版日期:2021-10-28 发布日期:2021-12-02
通讯作者: Yajie Tian, Guozhu Liu
基金资助:
Financial supports by the National Natural Science Foundation of China (21776210 and 22008055) are gratefully acknowledged.

Controllably tailoring external surface sites of nanosheet HZSM-5 for maximizing light olefins in catalytic cracking of n-decane

Tiantian Zhu¹, Hairui Liang¹, Bofeng Zhang¹, Yajie Tian², Guozhu Liu¹

1. Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
2. Henan Province Engineering Research Center of Catalytic Reaction, College of Chemistry and Chemical Engineering, Henan University, Kaifeng 475004, China

Received:2021-02-10 Revised:2021-04-04 Online:2021-10-28 Published:2021-12-02
Contact: Yajie Tian, Guozhu Liu
Supported by:
Financial supports by the National Natural Science Foundation of China (21776210 and 22008055) are gratefully acknowledged.

摘要/Abstract

摘要： A series of triphenylethoxysilane (TPEOS)-modified nanosheet HZSM-5 catalysts (ZN-x, x = 4%, 8% and 16%, mass) were synthesized by chemical liquid deposition to selectively change external acidity distributions. TPEOS modification was found to passivate some external Brønsted and Lewis acid sites by 37.8%, in which Brønsted acid sites (BAS) were found more easily sacrificed by breaking the surface AlO bond of bridging hydroxyl groups and forming SiOSi bonds. The selectivity of ZN-8 catalyst for light olefins (ethylene, propylene and butene) in n-decane catalytic cracking is up to 26% (450 ℃, WHSV = 10.95 h^-1), which is ca. 78% higher than that of parent one. The better performance was attributed to the appropriate external acid density in ZN-8, which inhibits bimolecular hydrogen transfer reaction of light olefins on the adjacent acid sites, resulting in more olefins, few coke precursors and thus an excellent catalytic stability.

关键词: Nanosheet HZSM-5, Acid properties, Surface modification, Catalysis, Deactivation, Fixed-bed

Abstract: A series of triphenylethoxysilane (TPEOS)-modified nanosheet HZSM-5 catalysts (ZN-x, x = 4%, 8% and 16%, mass) were synthesized by chemical liquid deposition to selectively change external acidity distributions. TPEOS modification was found to passivate some external Brønsted and Lewis acid sites by 37.8%, in which Brønsted acid sites (BAS) were found more easily sacrificed by breaking the surface AlO bond of bridging hydroxyl groups and forming SiOSi bonds. The selectivity of ZN-8 catalyst for light olefins (ethylene, propylene and butene) in n-decane catalytic cracking is up to 26% (450 ℃, WHSV = 10.95 h^-1), which is ca. 78% higher than that of parent one. The better performance was attributed to the appropriate external acid density in ZN-8, which inhibits bimolecular hydrogen transfer reaction of light olefins on the adjacent acid sites, resulting in more olefins, few coke precursors and thus an excellent catalytic stability.

Key words: Nanosheet HZSM-5, Acid properties, Surface modification, Catalysis, Deactivation, Fixed-bed

Tiantian Zhu, Hairui Liang, Bofeng Zhang, Yajie Tian, Guozhu Liu. Controllably tailoring external surface sites of nanosheet HZSM-5 for maximizing light olefins in catalytic cracking of n-decane[J]. 中国化学工程学报, 2021, 38(10): 276-285.

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Controllably tailoring external surface sites of nanosheet HZSM-5 for maximizing light olefins in catalytic cracking of n-decane

Controllably tailoring external surface sites of nanosheet HZSM-5 for maximizing light olefins in catalytic cracking of n-decane

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