Abstract
Quantum mechanical analysis reveals that carbonyl reduction of aldehydes and ketones by the imine-based reductant cis-[Os(III)(tpy)(Cl)(NH═CHCH(3))(NSAr)] (2), which is accessible by reduction of the analogous nitrile, occurs by hydride-proton transfer (HPT) involving both the imine and sulfilimido ligands. In carbonyl reduction, water or alcohol is necessary to significantly lower the barrier for proton shuttling between ligands. The -N(H)SAr group activates the carbonyl group through hydrogen bonding while the -NC(H)CH(3) ligand delivers the hydride.
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