Science · 2019 · 303 citations · 57 references
Natural SciencesChemistryMedicinal ChemistryCatalysisOrganic ChemistrySynthetic Medicinal ChemistryCatalyst DesignCross-coupling ReactionsHeterocyclic ChemistryOrganic SynthesisReaction MechanismsC - H Bond FunctionalizationCarbene Insertion ReactionsCarbon-heteroatom Bond FormationEnantioselective Catalyst DesignEnantioselective SynthesisSelectivity
Aliphatic amines strongly coordinate, and therefore easily inhibit, the activity of transition-metal catalysts, posing a marked challenge to nitrogen-hydrogen (N-H) insertion reactions. Here, we report highly enantioselective carbene insertion into N-H bonds of aliphatic amines using two catalysts in tandem: an achiral copper complex and chiral amino-thiourea. Coordination by a homoscorpionate ligand protects the copper center that activates the carbene precursor. The chiral amino-thiourea catalyst then promotes enantioselective proton transfer to generate the stereocenter of the insertion product. This reaction couples a wide variety of diazo esters and amines to produce chiral α-alkyl α-amino acid derivatives.
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Yan Zhao, Donald G. Truhlar · Theoretical Chemistry Accounts · 2007 · 30K citations · Full text
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Aleksandr V. Marenich, Christopher J. Cramer, Donald G. Truhlar · The Journal of Physical Chemistry B · 2009 · 17.4K citations · Full text
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Accurate Coulomb-fitting basis sets for H to Rn
Florian Weigend · Physical Chemistry Chemical Physics · 2006 · 8.8K citations
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