Vanadium(V) imido chlorides and n-propoxides — Towards a rational design of vanadium imido precatalysts for ethylene polymerization

Kayda, A.S.; Rumyantsev, A.V.; Zubkevich, S.V.; Zhizhko, P.A.; Takazova, R.U.; Tuskaev, V.A.; Gagieva, S.C.; Buzin, M.I.; Shatokhin, S.S.; Nikiforova, G.G.; Vasil'ev, V.G.; Pavlov, A.A.; Saracheno, D.; Melnikova, E.K.; Magomedov, K.F.; Kolosov, N.A.; Bulychev, B.M.

Авторы: Kayda Anatoliy S., Rumyantsev Andrey V., Zubkevich Sergey V., Zhizhko Pavel A., Takazova Rina U., Tuskaev Vladislav A., Gagieva Svetlana Ch, Buzin Mihail I., Shatokhin Stanislav S., Nikiforova Galina G., Vasil'ev Viktor G., Pavlov Alexander A., Saracheno Daniele, Melnikova Elizaveta K., Magomedov Kasim F., Kolosov Nikolay A., Bulychev Boris M.
Журнал: Journal of Organometallic Chemistry
Том: 934
Год издания: 2021
Издательство: Elsevier BV
Местоположение издательства: Netherlands
Номер статьи: 121665
DOI: 10.1016/j.jorganchem.2020.121665
Аннотация: Vanadium(V) imido complexes are widely used in olefin polymerization and oligomerization. In this re- port we present the synthesis and the results of ethylene polymerization studies for a series of vana- dium(V) imido complexes with various substituents at the imido fragment. All complexes have been prepared in nearly quantitative yields by the interaction of N -sulfinylamines with VOCl 3 or VO(O n Pr) 3 and characterized using 1 H, 13 C, 51 V NMR and elemental analysis. The solid-state structure of complex V( = NAr OMe )(O n Pr) 3 was established using X-ray. Vanadium(V) imido chlorides and n- propoxides exhibited similar moderate catalytic activities (320–547 kg PE ·mol(V) −1 ·h −1 ·atm −1 ). The maximum catalytic activity (547 kg PE ·mol(V) −1 ·h −1 ·atm −1 ) was achieved for (adamantylimido)vanadium(V) n -propoxide. The molec- ular weights of the resulting polyethylenes were higher (M v = 3.7–6.5 ·10 5 Da) for imido n- propoxide complexes as compared to the corresponding imido chlorides (M v = 2.1–5.5 ·10 5 Da). The localization of DFT calculated HOMO on imide nitrogen was proposed to favor the reaction between imide ligand and Et 2 AlCl used as activator.
Добавил в систему: Зубкевич Сергей Вадимович

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