Aseries of Mn I complexes containing lutidine-based chiral pincer ligands with modular and tunable structures has been developed. The complex shows unprecedentedly high activities (up to 9800 TON; TON = turnover number), broad substrate scope (81 examples), good functional-group tolerance,a nd excellent enantioselectivities (85-98 %e e) in the hydrogenation of various ketones.T hese aspects are rare in earth-abundant metal catalyzedhydrogenations.T he utility of the protocol have been demonstrated in the asymmetric synthesis of av ariety of key intermediates for chiral drugs. Preliminary mechanistic investigations indicate that an outersphere mode of substrate-catalyst interactions probably dominates the catalysis.Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.
Aseries of Mn I complexes containing lutidine-based chiral pincer ligands with modular and tunable structures has been developed. The complex shows unprecedentedly high activities (up to 9800 TON; TON = turnover number), broad substrate scope (81 examples), good functional-group tolerance,a nd excellent enantioselectivities (85-98 %e e) in the hydrogenation of various ketones.T hese aspects are rare in earth-abundant metal catalyzedhydrogenations.T he utility of the protocol have been demonstrated in the asymmetric synthesis of av ariety of key intermediates for chiral drugs. Preliminary mechanistic investigations indicate that an outersphere mode of substrate-catalyst interactions probably dominates the catalysis.Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.
A practical route from oxetane or thietane to γ-(thio)butyrolactone via solvated-proton-assisted cobalt-catalyzed carbonylative ring expansion under syngas atmosphere has been established. A wide variety of γ-(thio)butyrolactones can be afforded in good to excellent yields. The versatility of this method has been well demonstrated in the synthesis of intermediates towards the natural product Arctigenin as well as the pharmaceuticals Baclofen and Montelukast. The observed promoting effect of glycol ether solvent has been rationally interpreted.
By using methanol as the hydrogen source and commercially available nickel complex as the catalyst, the hydroarylative and hydroalkenylative cyclization of unsymmetrically substituted 1,6-dienes with organoboronic acid was developed to afford products with high regio- and diastereoselectivities.
Synthesis
of optically active gem-difluorinated organic molecules attracts a great deal of
interest due to their unique properties in pharmaceutical and agrochemical
areas. Herein, a series of enantioenriched α,α-difluoro-β-arylbutanoic
esters were prepared in high yields (83–99%) with moderate
to excellent enantioselectivities (≤97:3 er) by palladium-catalyzed
asymmetric hydrogenation.
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