Experimental and Theoretical Insights into the Electronic Properties of Anionic N-Heterocyclic Dicarbenes through the Rational Synthesis of Their Transition Metal Complexes

Grineva, A.A.; Filippov, O.A.; Canac, Y.; Sortais, J.; Nefedov, S.E.; Lugan, N.; César, V.; Valyaev, D.A.

Статья опубликована в высокорейтинговом журнале

Информация о цитировании статьи получена из Web of Science, Scopus
Статья опубликована в журнале из списка Web of Science и/или Scopus
Дата последнего поиска статьи во внешних источниках: 29 апреля 2021 г.

Авторы: Grineva Alina A., Filippov Oleg A., Canac Yves, Sortais Jean-Baptiste, Nefedov Sergei E., Lugan Noël, César Vincent, Valyaev Dmitry A.
Журнал: Inorganic Chemistry
Том: 60
Номер: 6
Год издания: 2021
Издательство: American Chemical Society
Местоположение издательства: United States
Первая страница: 4015
Последняя страница: 4025
Номер статьи: acs.inorgchem.1c00073
DOI: 10.1021/acs.inorgchem.1c00073
Аннотация: The lithiation of the NHC ligand backbone in Cp(CO)2Mn(IMes) followed by transmetalation on the C4 carbenic position with Cp(CO)2FeI led to the heterobimetallic complex Cp(CO)2Mn(μ-dIMes)Fe(CO)2Cp bearing the anionic ditopic imidazol-2,4-diylidene dIMes ligand. Subsequent treatment of the later with TfOH induced a selective decoordination of the [Cp(CO)2Mn] fragment to form the cationic abnormal NHC complex [Cp(CO)2Fe(aIMes)](OTf), which was further derivatized to the bis(iron) dIMes complex [Cp(CO)2Fe(μ-dIMes)Fe(CO)2Cp](OTf) by reaction with tAmOK and Cp(CO)2FeI. The effect of the metalation at the C4 or C2 position on the imidazole ring on the electronic donation properties of the associated C2 and C4 carbenic centers in the dIMes ligand was quantified through systematic experimental and theoretical studies of IMes, aIMes, and dIMes complexes. The evaluation of the catalytic activity of the series of cationic Fe(II) complexes based on IMes, aIMes, and dIMes ligands in a benchmark ketone hydrosilylation showed the superiority of the bimetallic derivative.
Добавил в систему: Астахов Григорий Сергеевич

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Experimental and Theoretical Insights into the Electronic Properties of Anionic N-Heterocyclic Dicarbenes through the Rational Synthesis of Their Transition Metal Complexesстатья

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