Mesoporous ZSM-5 zeolite catalysts prepared by desilication with organic hydroxides and comparison with NaOH leaching

沸石 介孔材料 煅烧 氢氧化物 浸出(土壤学) 催化作用 无机化学 化学 水溶液 溶解 化学工程 材料科学 有机化学 土壤水分 土壤科学 工程类 环境科学
作者
Sònia Abelló,Adriana Bonilla,Javier Pérez-Ramı́rez
出处
期刊:Applied Catalysis A-general [Elsevier BV]
卷期号:364 (1-2): 191-198 被引量:303
标识
DOI:10.1016/j.apcata.2009.05.055
摘要

Hierarchical zeolites combining micro- and mesoporosity were prepared by desilication of ZSM-5 (Si/Al = 42) in aqueous solutions of tetraalkylammonium hydroxides (TPAOH, TBAOH). Similarities between the treatment mediated by organic hydroxides and the conventional NaOH leaching comprised (i) the requirement to work with a starting zeolite in the optimal Si/Al window of 25–50 and (ii) the minor influence of the counter-cation (H+, NH4+, Na+) on the degree of mesoporosity developed. However, both desilication media presented distinctive kinetic and mechanistic characteristics. The use of organic hydroxides directly produced the protonic form of the mesoporous zeolite upon calcination, simplifying the final ion exchange with NH4NO3 characteristic of the NaOH treatment. Silicon dissolution in TPAOH (or TBAOH) was much slower than in NaOH, making the demetallation process highly controllable. The treatment in the organic base was less selective for silicon extraction, i.e. a higher amount of aluminum was leached to the solution compared to the NaOH treatment. The differences in porosity development and chemical composition of the final solid can be assigned to the effect of the bulky tetraalkylammonium cation. The optimal hierarchical ZSM-5 zeolite (treated in 1 M TPAOH at 338 K and 8 h) had a mesopore surface area of 160 m2 g−1 and the intrinsic zeolite properties were largely preserved. This sample displayed improved catalytic performance in the liquid-phase benzene alkylation with ethylene compared to the parent and NaOH-treated zeolites.
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