SuFEx wird biologisch: Biokompatible SOF4‐basierte SuFEx‐Reaktionen, die bei niedriger Konzentration in wässriger Lösung unter milden pH‐ und Temperaturbedingungen ablaufen, bieten Zugang zu asymmetrischen und am Schwefel(VI)‐Zentrum trisubstituierten Produkten mit vielseitiger S‐N‐ und S‐O‐Konnektivität. Die SuFEx‐Biokonjugation von Iminosulfuroxydifluoriden mit BSA‐Protein oder einzelsträngiger DNA wird demonstriert. Einzelheiten finden sich in der Zuschrift von K. B. Sharpless et al. auf S. 8113.
The oxidative coupling between two carbon–hydrogen (C–H) bonds offers the most straightforward pathway to construct C–C bonds from hydrocarbons without pre-functionalization, exhibiting high step- and atom-economy.
The activation of dinitrogen (N 2 ) and direct incorporation of its N atom into C−H bonds to create aliphatic C−N compounds remains unresolved. Incompatible conditions between dinitrogen reduction and C−H functionalization make this process extremely challenging. Herein, we report the first example of dinitrogen insertion into an aliphatic Csp 3 −H bond on the ligand scaffold of a 1,3-propane-bridged [N 2 N] 2− -type dititanium complex. Mechanistic investigations on the behaviors of dinuclear and mononuclear Ti complexes indicated the intramolecular synergistic effect of two Ti centers at a C−N bond-forming step. Computational studies revealed the critical isomerization between the inactive side-on N 2 complex and the active nitridyl complex, which is responsible for the Csp 3 −H amination. This strategy maps an efficient route toward the future synthesis of aliphatic amines directly from N 2 .
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