Nitrogenase Model Complexes [CpFe(μ-SR1)2(μ-η2-R2N=NH)FeCp] (R1 = Me, Et; R2 = Me, Ph; Cp* = η5-C5Me5): Synthesis, Structure, and Catalytic N-N Bond Cleavage of Hydrazines on Diiron Centers

被引：98

作者：

Chen, Yanhui ^{[1
]}

Zhou, Yuhan ^{[1
]}

Chen, Pingping ^{[1
]}

Tao, Yinsong ^{[1
]}

Li, Yang ^{[1
]}

Qu, Jingping ^{[1
]}

机构：

[1] Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, Dalian 116012, Peoples R China

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2008年 / 130卷 / 46期

基金：

中国国家自然科学基金;

关键词：

D O I：

10.1021/ja805025w

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The reactions of [Cp*Fe(mu-SR1)(3)FeCp*] (Cp* = eta(5)-C5Me5; R-1 = Et, Me) with 1.5 equiv (RNHNH2)-N-2 (R-2 = Ph, Me) give the mu-eta(2)-diazene diiron thiolate-bridged complexes [Cp*Fe(mu-SR1)(2)(mu-eta(2)-(RN)-N-2 NH)FeCp*], along with the formation of PhNH2 and NH3. These mu-eta(2)-diazene diiron thiolate-bridged complexes exhibit excellent catalytic N-N bond cleavage of hydrazines under ambient conditions.

引用

页码：15250 / +

页数：3

共 40 条

[1] Iron-sulfur clusters: Nature's modular, multipurpose structures [J].

Beinert, H ;

Holm, RH ;

Munck, E .

SCIENCE, 1997, 277 (5326) :653-659

[2] 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

[3] Mechanism of molybdenum nitrogenase [J].

Burgess, BK ;

Lowe, DJ .

CHEMICAL REVIEWS, 1996, 96 (07) :2983-3011

[4] Synthesis and reactions of novel triply thiolate-bridged diiron complexes [Cp*Fe(μ2-SR)3FeCp*] (Cp* = η5-C5Me5; R = Et, Ph) [J].

Chen, Yanhui ;

Zhou, Yuhan ;

Qu, Jingping .

ORGANOMETALLICS, 2008, 27 (04) :666-671

[5] Functional analogs for the reduction of certain nitrogenase substrates. Are multiple sites within the Fe/Mo/S active center involved in the 6e(-) reduction of N-2? [J].

Coucouvanis, D .

JOURNAL OF BIOLOGICAL INORGANIC CHEMISTRY, 1996, 1 (06) :594-600

[6] THE CATALYTIC REDUCTION OF HYDRAZINE TO AMMONIA BY THE MOFE3S4 CUBANES AND IMPLICATIONS REGARDING THE FUNCTION OF NITROGENASE - EVIDENCE FOR DIRECT INVOLVEMENT OF THE MOLYBDENUM ATOM IN SUBSTRATE REDUCTION [J].

COUCOUVANIS, D ;

MOSIER, PE ;

DEMADIS, KD ;

PATTON, S ;

MALINAK, SM ;

KIM, CG ;

TYSON, MA .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1993, 115 (25) :12193-12194

[7] The mechanistically significant coordination chemistry of dinitrogen at FeMo-co, the catalytic site of nitrogenase [J].

Dance, Ian .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2007, 129 (05) :1076-1088

[8]

EADY RR, 2007, CHEM-ASIAN J, V2, P936

[9] Nitrogenase MoFe-protein at 1.16 Å resolution:: A central ligand in the FeMo-cofactor [J].

Einsle, O ;

Tezcan, FA ;

Andrade, SLA ;

Schmid, B ;

Yoshida, M ;

Howard, JB ;

Rees, DC .

SCIENCE, 2002, 297 (5587) :1696-1700

[10] The first side-on bound metal complex of diazene, HN=NH [J].

Field, Leslie D. ;

Li, Hsiu L. ;

Dalgarno, Scott J. ;

Turner, Peter .

CHEMICAL COMMUNICATIONS, 2008, (14) :1680-1682

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Nitrogenase Model Complexes [Cp*Fe(μ-SR1)2(μ-η2-R2N=NH)FeCp*] (R1 = Me, Et; R2 = Me, Ph; Cp* = η5-C5Me5): Synthesis, Structure, and Catalytic N-N Bond Cleavage of Hydrazines on Diiron Centers

Nitrogenase Model Complexes [CpFe(μ-SR1)2(μ-η2-R2N=NH)FeCp] (R1 = Me, Et; R2 = Me, Ph; Cp* = η5-C5Me5): Synthesis, Structure, and Catalytic N-N Bond Cleavage of Hydrazines on Diiron Centers