Development of ruthenium(II) bis(N-Heterocyclic Carbene) complexes for homogeneous catalysis

IF 3.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis Pub Date : 2025-03-21 DOI:10.1016/j.mcat.2025.115032

Filippo Campagnolo, Eleonora Aneggi, Walter Baratta, Daniele Zuccaccia

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引用次数: 0

Abstract

A tetrakis(acetonitrile) complex bearing a bidentate bis(N-Heterocyclic Carbene) ligand was synthesized, and its formation was extensively studied. Triethylamine played a pivotal role in the reaction, initially forming a ruthenium(II)-triethylamino complex with the precursor. It then functioned as a base to produce the ruthenium(II) bis(NHC) complex, which was found to be very active in catalyzing the direct ortho-arylation of 2-phenylpyridine, with loadings as low as 2 % (a significant result considering that most reported examples in the literature require loadings as high as 10 % and are typically limited to monoarylations). Additionally, the reactive complex was successfully functionalized with various bidentate ligands of the amino, pyridine, and phosphine types, yielding a series of novel ruthenium(II) bis(NHC) dicationic organonitrile complexes. These complexes were evaluated in the catalytic transfer hydrogenation reaction, demonstrating notable activity (TOF of 50,000 h^-1). It is notable that within the pool of reported ruthenium(II) complexes featuring bidentate bis(NHC) ligands, cis- [Ru(CH₃CN)₂(1,1′-bis(3-methyl-imidazol-2-ylidene)methylene))(2–2′Bipyridine)](PF₆)₂ demonstrates exceptional high rate, marking it as one of the fastest known. Overall, the synthesized tetrakis(acetonitrile) complex proves to be a promising platform for the development of future catalysts.

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来源期刊

Molecular Catalysis Chemical Engineering-Process Chemistry and Technology

CiteScore

6.90

自引率

10.90%

发文量

700

审稿时长

40 days

期刊介绍： Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods