Highly para-selective alkylation of toluene by methyl mercaptan over silylated ZSM-5 zeolite

IF 6.5 1区化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-10-28 DOI:10.1016/j.jcat.2024.115828

Abdelilah Bayout , Claudia Cammarano , Izabel Medeiros Costa , Gleb Veryasov , Alexander Sachse , Vasile Hulea

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Abstract

Friedel-Crafts alkylation of toluene with methyl mercaptan has been investigated in the presence of H-ZSM-5 and SiO₂/H-ZSM-5 catalysts. The silica layers have been built on H-ZSM-5 zeolite by chemical liquid deposition of tetraethyl orthosilicate. The passivation with silica of the external surface of H-ZSM-5 zeolite has been confirmed by FT-IR spectroscopy and mesitylene isomerization, used as a model reaction. All catalysts exhibited notable behavior in the alkylation of toluene to xylenes. Efficiencies higher than 98 % in alkylation for both toluene and methyl mercaptan were obtained at 375 °C. In terms of para-selectivity, outstanding performance was revealed by the silylated zeolites. Thus, over 12 % SiO₂/H-ZSM-5, at 375 °C and WHSV = 9.4 g_{toluene+CH3SH} g_cat^-1h⁻¹, the para-xylene selectivity was close to 100 %. The experimental apparent activation energy for the toluene alkylation with methyl mercaptan catalyzed by H-ZSM-5 was 80 kJ/mol.

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硅烷化 ZSM-5 沸石上甲基硫醇对甲苯的高副选择性烷基化反应

在 H-ZSM-5 和 SiO2/H-ZSM-5 催化剂存在下，研究了甲苯与甲硫醇的 Friedel-Crafts 烷基化反应。H-ZSM-5 沸石上的二氧化硅层是通过正硅酸四乙酯的化学液相沉积而形成的。H-ZSM-5 沸石外表面的二氧化硅钝化已通过傅立叶变换红外光谱和用作模型反应的间苯异构化得到证实。在甲苯烷基化为二甲苯的过程中，所有催化剂都表现出了显著的性能。在 375 °C 时，甲苯和甲硫醇的烷基化效率均高于 98%。就副选择性而言，硅烷化沸石的性能十分突出。因此，在 375 ℃ 和 WHSV = 9.4 gtoluene+CH3SH gcat-1h-1 条件下，12 % SiO2/H-ZSM-5 的对二甲苯选择性接近 100%。H-ZSM-5 催化甲苯与甲硫醇发生烷基化反应的实验表观活化能为 80 kJ/mol。

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来源期刊

Journal of Catalysis 工程技术-工程：化工

CiteScore

12.30

自引率

5.50%

发文量

447

审稿时长

31 days

期刊介绍： The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.