Phosphido- and Amidozirconocene Cation-Based Frustrated Lewis Pair Chemistry

被引：64

作者：

Normand, Adrien T. ^{[1
,2
]}

Daniliuc, Constantin G. ^{[1
]}

Wibbeling, Birgit ^{[1
]}

Kehr, Gerald ^{[1
]}

Le Gendre, Pierre ^{[2
]}

Erker, Gerhard ^{[1
]}

机构：

[1] Univ Munster, Inst Organ Chem, D-48149 Munster, Germany

[2] Univ Bourgogne Franche Comte, Univ Bourgogne, CNRS, Inst Chim Mol,ICMUB UMR6302, F-21000 Dijon, France

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2015年 / 137卷 / 33期

关键词：

ORGANOLANTHANIDE-CATALYZED HYDROAMINATION; ZIRCONOCENE-PHOSPHINOARYLOXIDE COMPLEXES; VERLEY-TYPE REDUCTION; CARBON-DIOXIDE; INTRAMOLECULAR HYDROPHOSPHINATION/CYCLIZATION; STRUCTURAL-CHARACTERIZATION; TERMINATED POLYETHYLENES; HYDROGEN ACTIVATION; MOLECULAR-STRUCTURE; METAL-PHOSPHIDO;

D O I：

10.1021/jacs.5b06551

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Methyl abstraction from neutral [Cp2ZrMe-(ERR')] complexes 1 (E = N, P; R, R' = alkyl, aryl) with either B(C6F5)(3) or [Ph3C][B(C6F5)(4)] results in the formation of [Cp2Zr(ERR')][X] complexes 2 (X- = MeB(C6F5)(3)(-), B-(C6F5)(4)(-)). The X-ray structure of amido complexes [Cp2Zr-(NPh2)][MeB(C6F5)(3)] (2d) and [Cp2Zr((NBuAr)-Bu-t)][B-(C6F5)(4)] (2e', Ar = 3,5-C6H3(CH3)(2)) is reported, showing a sterically dependent Zr/N-pi interaction. Complexes 2 catalyze the hydrogenation of electron-rich olefins and alkynes under mild conditions (room temperature, 1.5 bar H-2). Complex 2e binds CO2, giving [Cp2Zr(CO2)((NBuAr)-Bu-t)](2)[MeB(C6F5)(3)](2) (3e). Amido complex 2d reacts with benzaldehyde yielding [Cp2Zr(OCH2Ph)((OC)PhNPh2)][MeB(C6F5)(3)] (7d). Phosphido complex [Cp2Zr(PCy2)] [MeB(C6F5)(3)] (2a) reacts with diphenylacetylene to yield frustrated Lewis pair [Cp2Zr(PhCCPh)(PCy2)] [MeB(C6F5)(3)] (8a) which further reacts with a range of carbonyl substrates.

引用

页码：10796 / 10808

页数：13

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