Design and Synthesis of Octahedral Metal Complexes with Linear Multidentate Ligands

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Asymmetric catalysis converts a prochiral substrate into an enantiomericallyenriched chiral product. The enantioselectivity has generally been interpreted as a result of competing diastereomorphic catalytic cycles involving a single chiral catalyst. We have designed and synthesized Ph-BINAN-H-Py which is characterized by i) inside sp^N/outside sp^N, ii) donor-acceptor bifunctional ability, and iii) cis-alpha-selective formation of octahedral metal complexes. The utility of ligands has been demonstrated in asymmetric hydrogenation of aromatic ketones in combination with a Ru-π-allyl precursor. A series of detailed mechanistic studies should stimulate our ideas for development of asymmetric molecular catalysis.