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Article Dans Une Revue Chemistry - A European Journal Année : 2021

Ruthenium-Catalyzed Coupling Reactions of CO2 with C2H4 and Hydrosilanes towards Silyl Esters

Résumé

A series of in situ-prepared catalytic systems incorporating RuII precursors and bidentate phosphine ligands has been probed in the reductive carboxylation of ethylene in the presence of triethylsilane as reductant. The catalytic production of propionate and acrylate silyl esters was evidenced by high-throughput screening (HTS) and implemented in batch reactor techniques. The most promising catalyst systems identified were made of Ru(H)(Cl)(CO)(PPh3)3 and 1,4-bis(dicyclohexylphosphino)butane (DCPB) or 1,1’-ferrocene-diyl-bis(cyclohexylphosphine) (DCPF). A marked influence of water on the acrylate/propionate selectivity was noted. Turnover numbers [mol mol(Ru)−1] up to 16 for acrylate and up to 68 for propionate were reached under relatively mild conditions (20 bar, 100 °C, 0.5 mol % Ru, 40 mol % H2O vs. HSiEt3). Possible mechanisms are discussed.
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Dates et versions

hal-03102186 , version 1 (26-01-2021)

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Kana Kunihiro, Svetlana Heyte, Paul Sébastien, Thierry Roisnel, Jean-François Carpentier, et al.. Ruthenium-Catalyzed Coupling Reactions of CO2 with C2H4 and Hydrosilanes towards Silyl Esters. Chemistry - A European Journal, 2021, 27 (12), pp.3997-4003. ⟨10.1002/chem.202005083⟩. ⟨hal-03102186⟩
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