Lutidine-Derived Ru-CNC Hydrogenation Pincer Catalysts with Versatile Coordination Properties

被引：96

作者：

Filonenko, Georgy A. ^{[1
,2
]}

Cosimi, Elena ^{[3
]}

Lefort, Laurent ^{[3
]}

Conley, Matthew P. ^{[4
]}

Coperet, Christophe ^{[4
]}

Lutz, Martin ^{[5
]}

Hensen, Emiel J. M. ^{[1
,2
]}

Pidko, Evgeny A. ^{[1
,2
]}

机构：

[1] Eindhoven Univ Technol, Inorgan Mat Chem Grp, Schuit Inst Catalysis, POB 513, NL-5600 MB Eindhoven, Netherlands

[2] Eindhoven Univ Technol, Inst Complex Mol Syst, NL-5600 MB Eindhoven, Netherlands

[3] DSM Innovat Synth BV, NL-6160 MD Geleen, Netherlands

[4] ETH, Dept Chem & Appl Biosci, CH-8093 Zurich, Switzerland

[5] Univ Utrecht, Bijvoet Ctr Biomol Res, NL-3584 CH Utrecht, Netherlands

来源：

ACS CATALYSIS | 2014年 / 4卷 / 08期

关键词：

ruthenium; hydrogenation; metal-ligand cooperation; N-heterocyclic carbene; nitrile activation; METAL-LIGAND COOPERATION; N-HETEROCYCLIC CARBENES; HETEROGENEOUS CATALYSIS; BOND FORMATION; RUTHENIUM(II) COMPLEXES; IMIDAZOLIUM SALT; IRON(II) COMPLEX; ESTERS; ACTIVATION; NITRILES;

D O I：

10.1021/cs500720y

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Lutidine-derived bis-N-heterocyclic carbene (NHC) ruthenium CNC-pincer complexes (Ru-CNC's) were prepared. Depending on the synthetic procedure, normal (1, 2) or mixed normal/abnormal NHC-complexes (3) are formed. In the presence of phosphazene base, Ru-CNC complexes activate nitriles to give ketimino compounds 4-6. Nitrile adduct 4 shows reactivity toward strong bases to yield dearomatized complex 7, which heterolytically activates H-2 to form the bis-hydrido complex 8. Finally, these Ru-CNC's are active in catalytic hydrogenation of CO2 to formate salts, and unlike the phosphine-containing Ru-PNP counterpart, they also catalyze the selective hydrogenation of esters to alcohols.

引用

页码：2667 / 2671

页数：5

共 32 条

[31] Protic- or anionic-NHCs with a classical-NHC in a single [Ru(CNC)(PPh3)2Cl]Cl pincer complex: direct comparison of structure & electronic properties and heterolytic H2 splitting
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[32] Metal carbonyl clusters as precursors of heterogeneous catalysts: Hydrogenation and disproportionation of monoenes, dienes, and arenes in the presence of H2Ru4(CO)13, H2FeRu3(CO)13, and HRuCo3(CO)12 supported and activated on chromosorb. Characterization of the metal particles derived from H2Ru4(CO)13 by means of IR spectroscopy and TEM microscopy
Mario Castiglioni
Stefano Deabate
Edoardo Garrone
Roberto Giordano
Barbara Onida
Giovanni Predieri
Enrico Sappa
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