期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 145, 期 12, 页码 6773-6780出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c13086
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This study reports the first example of dinitrogen insertion into an aliphatic Csp3-H bond on the ligand scaffold of a 1,3-propane-bridged dititanium complex. Mechanistic investigations revealed the intramolecular synergistic effect of two Ti centers at a C-N bond-forming step. This strategy provides an efficient route for the future synthesis of aliphatic amines directly from N2.
The activation of dinitrogen (N2) 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 Csp3-H bond on the ligand scaffold of a 1,3-propane-bridged [N2N]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 N2 complex and the active nitridyl complex, which is responsible for the Csp3-H amination. This strategy maps an efficient route toward the future synthesis of aliphatic amines directly from N2.
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