Lutidine-derived Ru-CNC hydrogenation pincer catalysts with versatile coordination properties

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Access status: Embargo until 2050-01-01 , cs500720y.pdf (1.06 MB)

Publication date

2014-01-01

Authors

Filonenko, Georgy A.
Cosimi, Elena
Lefort, Laurent
Conley, Matthew P.
Copéret, Christophe
Lutz, MartinORCID 0000-0003-1524-9629ISNI 0000000352600916
Hensen, Emiel J M
Pidko, Evgeny A.

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Abstract

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 H2 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.

Keywords

hydrogenation, metal-ligand cooperation, N-heterocyclic carbene, nitrile activation, ruthenium, Catalysis

Citation

Filonenko, G A, Cosimi, E, Lefort, L, Conley, M P, Copéret, C, Lutz, M, Hensen, E J M & Pidko, E A 2014, 'Lutidine-derived Ru-CNC hydrogenation pincer catalysts with versatile coordination properties', ACS Catalysis, vol. 4, no. 8, pp. 2667-2671. https://doi.org/10.1021/cs500720y