Journal of the American Chemical Society p. 6794 - 6800 (1986)
Update date:2022-08-10
Topics:
Sheldon, John C.
Bowie, John H.
DePuy, Charles H.
Damrauer, Robert
The ions H3Si- and Me3Si- undergo Si-O and/or Si-S bond forming reactions with CO2, COS, CS2, SO2, N2O, MeNCO, and MeNCS forming H3SiO3-, Me3SiO-, H3SiS-, or Me3SiS- ions as appropriate.The rates of these reactions vary markedly, e.g., the reaction of H3Si- with CS2 (to form H3SiS- + CS) occurs at every encounter, whereas that of H3Si- with N2O (to form H3SiO- plus N2) occurs for only one in every thousand collisions.Ab initio calculations (at 6-31G level) for the reactions of H3Si- with CO2, CS2, SO2, and N2O suggest different and complex reaction pathways.The reaction of H3Si- with CO2 is characterized by initial approach to carbon, and subsequent rearrangements are required to form H3SiO-.H3SiS- is formed by a simple path from CS2 following initial attack at sulfur.H3Si- reacts with SO2 in alternative ways to form five-coordinate intermediate which subsequently decomposes to H3SiO- plus SO.H3Si- is likely to attack N2O at the terminal nitrogen, and subsequent rearrangement forms H3SiO-.The length, or complexity of the reaction pathway appears inversely related to the measured efficiency in the majority of reactions.
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