期刊
INORGANICA CHIMICA ACTA
卷 518, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.ica.2021.120257
关键词
N-ligands; Schiff bases; Polymeric ligands; Ruthenium; Heterogenized catalysts
资金
- Universit`a degli Studi di Milano
The use of polymer-immobilized catalysts can enhance recovery efficiency but may also lead to reduced catalytic activity. By adjusting the structure of the polymer, a balance between catalytic activity and recovery efficiency can be achieved.
Use of homogeneous catalysts poses the problem of their recovery at the end of the reaction. A possible strategy to circumvent this problem is to make the ligand part of a polymer with limited solubility. In this work, we investigated the immobilization of complexes of Ar-BIAN ligands (Ar-BIAN = bis(arylimido)acenaphthene). We employed 4,4'-methylene-bis(aniline) as an amine able to bridge two acenaphthene moieties. However, the obtained product was a mixture of short-chain oligomers. A ruthenium complex of this mixture (Oligo-BIAN) was indeed catalytically active in the model hydrogenation of nitrobenzene to aniline by CO/H2O but the complexes were too soluble in the reaction mixture to allow for an easy recovery. We thus further extended the molecular weight of Oligo-BIAN by polymerizing it with terephthaloyl chloride obtaining a polyamide (Poly-BIAN). The latter was insoluble in all solvents but its ruthenium complex was catalytically inactive in the model reaction. An deeper investigation, showed that coordination mode of monomeric Ar-BIAN ligands and Oligo-BIAN to [Ru (CO)(3)Cl-2(THF)] is differs from that of Poly-BIAN. This result was completely unexpected and constitutes a general warning not to give for granted the coordination mode of a complex to a functionalized polymer.
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