Silyl carbamates were synthesized from amines, carbon dioxide and hydrosilanes using Ir–NSiN complexes. Iridium complex [Ir(H)(CF3SO3)(NSiN)(coe)] (NSiN=bis(pyridine-2-yloxy)methylsilyl) is proved to be effective catalyst precursor for the solvent-free synthesis of silyl carbamates and this work constitutes a first example using Iridium catalyst. The expected product from the reaction of amines, CO2 and silane was formamide or methylamine. Surprisingly, iridium-catalyzed dehydrogenative Si-N coupling between the silane and the amine was happened which afford the corresponding silyl amine. Then, silyl amine reacts with CO2 under the reaction conditions to give the corresponding silyl carbamate. Theoretical and experimental calculations suggest that a competition between both hydrosilylation of CO2 and dehydrogenative coupling reactions of amine–silane controls the selectivity of the process. 

Reactivity of CO<sub>2</sub> with secondary amines and hydrosilanes using Ir���NSiN Complexes

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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Reactivity of CO2 with secondary amines and hydrosilanes using Ir���NSiN Complexes

Reactivity of CO₂ with secondary amines and hydrosilanes using Ir��NSiN Complexes