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

Abstract

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

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

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]. Chinese Journal of Chemical Engineering, 2021, 38(10): 276-285.

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