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The final products of the reaction with CS<jats:sub>2<\/jats:sub> are methane and the previously unknown [(Et<jats:sub>3<\/jats:sub>Si)<jats:sub>3<\/jats:sub>S]<jats:sup>+<\/jats:sup> cation. To gain insight into the entire reaction cascade, numerous experiments with varying conditions were performed, intermediate products were intercepted, and their structures were determined by X\u2010ray crystallography. Besides the [(Et<jats:sub>3<\/jats:sub>Si)<jats:sub>3<\/jats:sub>S]<jats:sup>+<\/jats:sup> cation as the final product, crystal structures of [(Et<jats:sub>3<\/jats:sub>Si)<jats:sub>2<\/jats:sub>SMe]<jats:sup>+<\/jats:sup>, [Et<jats:sub>3<\/jats:sub>SiS(H)Me]<jats:sup>+<\/jats:sup>, and [Et<jats:sub>3<\/jats:sub>SiOC(H)OSiEt<jats:sub>3<\/jats:sub>]<jats:sup>+<\/jats:sup> were obtained. Experimental results combined with supporting quantum\u2010chemical calculations in the gas phase and solution allow a detailed understanding of the reaction cascade.<\/jats:p>","DOI":"10.1002\/chem.202005003","type":"journal-article","created":{"date-parts":[[2020,11,20]],"date-time":"2020-11-20T16:21:12Z","timestamp":1605889272000},"page":"3288-3291","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":8,"title":["Activation of CS<sub>2<\/sub> and CO<sub>2<\/sub> by Silylium Cations"],"prefix":"10.1002","volume":"27","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5913-3989","authenticated-orcid":false,"given":"Carsten","family":"Jenne","sequence":"first","affiliation":[{"name":"Anorganische Chemie Fakult\u00e4t f\u00fcr Mathematik und Naturwissenschaften Bergische Universit\u00e4t Wuppertal  Gau\u00dfstr. 20 42119 Wuppertal 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