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Benzoimidazole-Pyridylamido Zirconium and Hafnium Alkyl Complexes as Homogeneous Catalysts for Tandem Carbon Dioxide Hydrosilylation to Methane

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dc.contributor.author Luconi L.
dc.contributor.author Rossin A.
dc.contributor.author Tuci G.
dc.contributor.author Gafurov Z.
dc.contributor.author Lyubov D.
dc.contributor.author Trifonov A.
dc.contributor.author Cicchi S.
dc.contributor.author Ba H.
dc.contributor.author Pham-Huu C.
dc.contributor.author Yakhvarov D.
dc.contributor.author Giambastiani G.
dc.date.accessioned 2020-01-15T21:56:24Z
dc.date.available 2020-01-15T21:56:24Z
dc.date.issued 2019
dc.identifier.issn 1867-3880
dc.identifier.uri https://dspace.kpfu.ru/xmlui/handle/net/156427
dc.description.abstract © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim Neutral Zr IV and Hf IV alkyl/amido complexes stabilized by a tridentate N ligand that contains a “rolling” heterodentate benzoimidazole fragment have been prepared and characterized. The ultimate nature of the ligand denticity, the electronic properties of the ligand binding pocket and the metal coordination environment are controlled by the protection/deprotection of the benzoimidazole NH group. The metal precursor used [M IV (Bn) 4 or M IV (NMe 2 ) 4 ] also has an influence on the final coordination sphere of the complex; indeed, a permanent central pyridine dearomatization occurs in the presence of dimethylamido ancillary groups. DFT calculations on the real system have been used to elucidate the mechanism. Selected alkyl species from this series have been scrutinized for the tandem hydrosilylation of CO 2 to CH 4 in combination with the strong Lewis acid B(C 6 F 5 ) 3 using a variety of hydrosilanes. A positive effect of the hardness modification of the ligand donor atom set is observed in the catalytic outcomes. Indeed, κ 3 {N − ,N,N − }Zr IV (Bn) 2 catalyzes the process to methane selectively with a turnover frequency as high as 272 h −1 (at 96 % substrate conversion) almost twice as much as that claimed for the benchmark κ 3 {O − ,O,O − }Zr IV (Bn) 2 complex under similar experimental conditions.
dc.relation.ispartofseries ChemCatChem
dc.subject hafnium
dc.subject homogeneous catalysis
dc.subject N ligands
dc.subject reduction
dc.subject zirconium
dc.title Benzoimidazole-Pyridylamido Zirconium and Hafnium Alkyl Complexes as Homogeneous Catalysts for Tandem Carbon Dioxide Hydrosilylation to Methane
dc.type Article
dc.relation.ispartofseries-issue 1
dc.relation.ispartofseries-volume 11
dc.collection Публикации сотрудников КФУ
dc.relation.startpage 495
dc.source.id SCOPUS18673880-2019-11-1-SID85059455244

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  • Публикации сотрудников КФУ Scopus [24551]
    Коллекция содержит публикации сотрудников Казанского федерального (до 2010 года Казанского государственного) университета, проиндексированные в БД Scopus, начиная с 1970г.

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