Abdelilah Bayout , Claudia Cammarano , Izabel Medeiros Costa , Gleb Veryasov , Alexander Sachse , Vasile Hulea
{"title":"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","authors":"Abdelilah Bayout , Claudia Cammarano , Izabel Medeiros Costa , Gleb Veryasov , Alexander Sachse , Vasile Hulea","doi":"10.1016/j.jcat.2024.115828","DOIUrl":null,"url":null,"abstract":"<div><div>Friedel-Crafts alkylation of toluene with methyl mercaptan has been investigated in the presence of H-ZSM-5 and SiO<sub>2</sub>/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 <em>para</em>-selectivity, outstanding performance was revealed by the silylated zeolites. Thus, over 12 % SiO<sub>2</sub>/H-ZSM-5, at 375 °C and WHSV = 9.4 g<sub>toluene+CH3SH</sub> g<sub>cat</sub><sup>-1</sup>h<sup>−1</sup>, the <em>para</em>-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.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115828"},"PeriodicalIF":6.5000,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Highly para-selective alkylation of toluene by methyl mercaptan over silylated ZSM-5 zeolite\",\"authors\":\"Abdelilah Bayout , Claudia Cammarano , Izabel Medeiros Costa , Gleb Veryasov , Alexander Sachse , Vasile Hulea\",\"doi\":\"10.1016/j.jcat.2024.115828\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Friedel-Crafts alkylation of toluene with methyl mercaptan has been investigated in the presence of H-ZSM-5 and SiO<sub>2</sub>/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 <em>para</em>-selectivity, outstanding performance was revealed by the silylated zeolites. Thus, over 12 % SiO<sub>2</sub>/H-ZSM-5, at 375 °C and WHSV = 9.4 g<sub>toluene+CH3SH</sub> g<sub>cat</sub><sup>-1</sup>h<sup>−1</sup>, the <em>para</em>-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.</div></div>\",\"PeriodicalId\":346,\"journal\":{\"name\":\"Journal of Catalysis\",\"volume\":\"440 \",\"pages\":\"Article 115828\"},\"PeriodicalIF\":6.5000,\"publicationDate\":\"2024-10-28\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0021951724005414\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0021951724005414","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Highly para-selective alkylation of toluene by methyl mercaptan over silylated ZSM-5 zeolite
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 gtoluene+CH3SH gcat-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.
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.
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