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• W2256750602 abstract "Hydrosilylation of C–C multiple bonds is one of the most important applications of homogeneous catalysis in industry. The reaction is characterized by its atom-efficiency, broad substrate scope, and widespread application. To date, industry still relies on highly active platinum-based systems that were developed over half a century ago. Despite the rapid evolution of vast synthetic applications, the development of a fundamental understanding of the catalytic reaction pathway has been difficult and slow, particularly for the industrially highly relevant Karstedt’s catalyst. A detailed mechanistic study unraveling several new aspects of platinum-catalyzed hydrosilylation using Karstedt’s catalyst as platinum source is presented in this work. A combination of 2H-labeling experiments, 195Pt NMR studies, and an in-depth kinetic study provides the basis for a further development of the well-established Chalk–Harrod mechanism. It is concluded that the coordination strength of the olefin exerts a decisive effect on the kinetics of the reaction. In addition, it is demonstrated how distinct structural features of the active catalyst species can be derived from kinetic data. A primary kinetic isotope effect as well as a characteristic product distribution in deuterium-labeling experiments lead to the conclusion that the rate-limiting step of platinum-catalyzed hydrosilylation is in fact the insertion of the olefin into the Pt–H bond rather than reductive elimination of the product in the olefin/silane combinations studied." @default.
• W2256750602 created "2016-06-24" @default.
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• W2256750602 date "2016-01-26" @default.
• W2256750602 modified "2023-10-06" @default.
• W2256750602 title "Platinum Catalysis Revisited—Unraveling Principles of Catalytic Olefin Hydrosilylation" @default.
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• W2256750602 doi "https://doi.org/10.1021/acscatal.5b02624" @default.
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