High-Spin Iron(I) and Iron(0) Dinitrogen Complexes Supported by N-Heterocyclic Carbene Ligands

被引：31

作者：

Ouyang, Zhenwu ^{[1
]}

Cheng, Jun ^{[1
]}

Li, Lingling ^{[2
]}

Bao, Xiaoli ^{[2
]}

Deng, Liang ^{[1
]}

机构：

[1] Chinese Acad Sci, Shanghai Inst Organ Chem, State Key Lab Organometall Chem, 345 Lingling Rd, Shanghai 200032, Peoples R China

[2] Shanghai Jiao Tong Univ, Instrumental Anal Ctr, 800 Dongchuan Rd, Shanghai 200240, Peoples R China

来源：

CHEMISTRY-A EUROPEAN JOURNAL | 2016年 / 22卷 / 40期

基金：

中国国家自然科学基金;

关键词：

FEMO-COFACTOR; MOLYBDENUM COFACTOR; C-ATOM; N-2; NITROGENASE; CARBON; CHEMISTRY; HYDRIDE; REDUCTION; BINDING;

D O I：

10.1002/chem.201603390

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The use of 1,3-dicyclohexylimidazol-2-ylidene (ICy) as ligand has enabled the preparation of the high-spin tetrahedral iron(I)- and iron(0)-N-2 complexes, namely [(ICy)(3)Fe(N-2)][BPh4] (1) and [(ICy)(3)Fe(N-2)] (2), the electronic structures of which have been established by various spectroscopic characterization and DFT calculations. The frequency of the N-N stretching resonance of the iron(0)N-2 complex is the lowest among the reported terminal N-2 complexes of iron, signifying the beneficial roles of strongly sigma-donating ligands in combination with the high-spin low-valent iron center in promoting N-2-activation. The iron(0)-N-2 complex can convert reversibly to the low-spin iron(II)-N-2 hydride complex [(ICy)(2)(ICy')Fe(N-2)(H)] (4).

引用

页码：14162 / 14165

页数：4

共 60 条

[1]

[Anonymous], 2015, BIOINSPIRED CATALYSI

[2] Selective Extraction of N2 from Air by Diarylimine Iron Complexes [J].

Bartholomew, Erika R. ;

Volpe, Emily C. ;

Wolczanski, Peter T. ;

Lobkovsky, Emil B. ;

Cundari, Thomas R. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2013, 135 (09) :3511-3527

[3] A tetrahedrally coordinated L3Fe-Nx platform that accommodates terminal nitride (FeIVN) and dinitrogen (FeI-N2-FeI) ligands [J].

Betley, TA ;

Peters, JC .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (20) :6252-6254

[4] Dinitrogen chemistry from trigonally coordinated iron and cobalt platforms [J].

Betley, TA ;

Peters, JC .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2003, 125 (36) :10782-10783

[5] Transition metal dinitrogen complexes supported by a versatile monoanionic [N2P2] ligand [J].

Chomitz, Wayne A. ;

Arnold, John .

CHEMICAL COMMUNICATIONS, 2007, (45) :4797-4799

[6] Insight into the Iron Molybdenum Cofactor of Nitrogenase from Synthetic Iron Complexes with Sulfur, Carbon, and Hydride Ligands [J].

Coric, Ilija ;

Holland, Patrick L. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2016, 138 (23) :7200-7211

[7] Binding of dinitrogen to an iron-sulfur-carbon site [J].

Coric, Ilija ;

Mercado, Brandon Q. ;

Bill, Eckhard ;

Vinyard, David J. ;

Holland, Patrick L. .

NATURE, 2015, 526 (7571) :96-99

[8] Catalytic Reduction of N2 to NH3 by an Fe-N2 Complex Featuring a C-Atom Anchor [J].

Creutz, Sidney E. ;

Peters, Jonas C. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (03) :1105-1115

[9] Iron-dinitrogen coordination chemistry: Dinitrogen activation and reactivity [J].

Crossland, Justin L. ;

Tyler, David R. .

COORDINATION CHEMISTRY REVIEWS, 2010, 254 (17-18) :1883-1894

[10] Molecular N2 complexes of iron stabilised by N-heterocyclic 'pincer' dicarbene ligands [J].

Danopoulos, AA ;

Wright, JA ;

Motherwell, WB .

CHEMICAL COMMUNICATIONS, 2005, (06) :784-786

← 1 2 3 4 5 6 →