Untangling the role of the organosilane functional groups in the synthesis of hierarchical ZSM-5 zeolite by crystallization of silanized protozeolitic units

• Published in: Catalysis today Vol. 345; pp. 27 - 38
• Main Authors: Alonso-Doncel, M., Peral, A., Shamzhy, M., Čejka, J., Sanz, R., Serrano, D.P.
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 01.04.2020
• Subjects: Catalytic cracking; Hierarchical zeolites; LDPE; Organosilane; Silanization; ZSM-5; Organosilane; Silanization; LDPE; Hierarchical zeolites; ZSM-5; Catalytic cracking
• ISSN: 0920-5861; 1873-4308
• DOI: 10.1016/j.cattod.2019.11.031

[Display omitted] •Amines and dipodal moieties favor organosilane-protozeolitic nanounits interactions.•Dipodal organosilanes produce non-completely crystalline ZSM-5 materials.•Organosilane combining phenyl and amine groups generate more uniform mesopores.•Uniform h-ZSM-5 properties lead to LDPE cracking in a narrow temperature range. Crystallization of hierarchical ZSM-5 zeolite has been performed under hydrothermal conditions from silanized protozeolitic units. The role of amine and phenyl groups present in the organosilanes, as well as the use of dipodal silanization agents, on the creation of mesoporosity in the zeolite samples has been investigated. The presence of amine groups and dipodal moieties in the organosilane increases their interactions with the protozeolitic nanounits in the gel, which results in hierarchical zeolites showing enhanced secondary porosity and a higher degree of modification of the textural properties. Nevertheless, dipodal organosilanes hinder strongly the aggregation of the nanounits, leading to non-completely crystalline materials. In contrast, the combination of phenyl and amine groups into a single organosilane has shown to be effective for the generation of more uniform mesopores. Thus, N-(2-N-Benzylaminoethyl)-3-aminopropyltrimethoxysilane (Ph-2A) has been found as the best silanization agent, affording a hierarchical zeolite with a narrow mesopore size distribution and a high concentration of strong Brønsted acid sites. Moreover, during LDPE catalytic cracking in TGA tests, the latter material allowed the conversion of the polymer to occur in a narrow temperature range as a consequence of its more uniform acid and textural properties. Likewise, this sample exhibited a high activity in LDPE cracking at 340 °C using a laboratory scale reaction system to produce mainly gasoline-range hydrocarbons and light olefins.