Repozytorium

A family of group 4 metal alkoxo complexes with an M33-O) core relevant to Ziegler-Natta catalyst intermediates.

Autorzy

Józef Utko

Szymon Przybylak

Lucjan B. Jerzykiewicz

Sławomir Szafert

Piotr Sobota

Rok wydania

2003

Czasopismo

Chemistry-A European Journal

Numer woluminu

9

Strony

181-190

DOI

10.1002/chem.200390011

Kolekcja

Naukowa

Język

Angielski

Typ publikacji

Artykuł

Streszczenie

Highly optimized syntheses of interesting model intermediates in Ziegler–Natta catalysis are described. These zirconium and hafnium alkoxo complexes have a stable (μ3-O)M3 core and incorporate an alkaline earth metal containing moiety, as illustrated. Their formation pathway gives an insight into the mechanism of Z–N procatalyst formation. Solvent polarity plays a pivotal role in formation of the final product. Reactions of [Mg(thffo)2] (1) or [Ca(thffo)2] (2) with ZrCl4 or HfCl4 in a CH2Cl2/THF/CH3CN mixture give thermall stable neutral heterobimetallic tetranuclear complexes [M3M′(μx-O)(μ,η2-thffo)6(Cl)6] (thffo=tetrahydrofurfuroxide; M/M′/x: 3, Zr/Mg/3; 4, Hf/Mg/3; 5, Zr/Ca/4; 6, Hf/Ca/4) as colorless crystals in 75–82 % yield. X-ray diffraction studies show complexes 35 to contain oxo-bridged M3 triangles that are capped by an alkaline earth metal-containing moiety to form species of C3 symmetry. Reactions of ZrCl4 and HfCl4 with pure tetrahydrofurfuryl alcohol in EtOH and MeOH provide ionic complexes [M3(μ3-O)(μ,η2-thffo)3(L)3(Cl)6]Cl (M/L: 8, Zr/EtOH; 9, Hf/EtOH; 10, Zr/MeOH) in 66–79 % yield. Complexes 810 consist of M3 triangles that are analogous to those in 36 and possess similar overall symmetry, as shown by X-ray crystallography. Changes in the reaction conditions afforded the asymmetric neutral dimer [Zr2(μ-thffo)2(thffoH)(Cl)6] (7) and the homometallic [Zr3(μ3-O)(μ,η2-thp)3(thf)2(Cl)7] (11).

Adres publiczny

https://doi.org/10.1002/chem.200390011

Strona internetowa wydawcy

onlinelibrary.wiley.com

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