Examining the Generality of Metal-Ligand Cooperativity Across a Series of First-Row Transition Metals: Capture, Bond Activation, and Stabilization

被引：16

作者：

Kiernicki, John J. ^{[1
]}

Zeller, Matthias ^{[2
]}

Szymczak, Nathaniel K. ^{[1
]}

机构：

[1] Univ Michigan, Dept Chem, Ann Arbor, MI 48109 USA

[2] Purdue Univ, Dept Chem, HC Brown Lab, W Lafayette, IN 47907 USA

来源：

INORGANIC CHEMISTRY | 2020年 / 59卷 / 13期

关键词：

COBALT COMPLEXES; ALKYL MIGRATION; IRON; COORDINATION; DINITROGEN; REDUCTION; CLEAVAGE; REACTIVITY; MECHANISM; AMMONIA;

D O I：

10.1021/acs.inorgchem.0c01163

中图分类号：

O61 [无机化学];

学科分类号：

070301 ; 081704 ;

摘要：

We outline the generality and requirements for cooperative N2H4 capture, N-N bond scission, and amido stabilization across a series of first-row transition metal complexes bearing a pyridine(dipyrazole) ligand. This ligand contains a pair of flexibly tethered trialkylborane Lewis acids that enable hydrazine capture and M-NH2 stabilization. While the Lewis acids are required to bind N2H4, the identity of the metal dictates whether N-N bond scission can occur. The redox properties of the M(II) bis(amidoborane) series of complexes were investigated and reveal that ligand-based events prevail; oxidation results in the generation of a transiently formed aminyl radical, while reduction occurs at the redox-active pyridine(dipyrazole) ligand.

引用

页码：9279 / 9286

页数：8

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