Publikation: Anion exchange in alkyl-zirconocene borate ion pairs : are solvated alkyl-zirconocene cations relevant intermediates?
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2001
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Journal of the American Chemical Society. 2001, 123(7), pp. 1483-1489. ISSN 0002-7863. eISSN 1520-5126. Available under: doi: 10.1021/ja003531w
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Ion pairs of the type Cpx2ZrMe+***A- containing various ansa-zirconocene methyl cations in contact with Me-B(C6F5)3- or B(C6F5)4- anions have been studied with regard to their anion exchange kinetics by 2D-NMR methods in benzene or toluene solutions. The resultsacceleration of anion exchange by added Li+***Me−B(C6F5)3-, substantial nonproductive exchange between added and Zr-bound Me-B(C6F5)3- anions, an increase of exchange rates at increased zirconocene concentrations, and the exclusively entropic origin of this rate increaseall indicate that anion exchange occurs by way of ion quadruples or higher ionic aggregates, rather than via dissociation to solvent-separated ions. These findings imply that solvent-separated (i.e. anion-free) alkyl zirconocene cations are unlikely to be relevant intermediates in reaction systems containing Cpx2ZrMe+***A- ion pairs and, hence, also in zirconocene-based catalyst systems for the polymerization of α-olefins.
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BECK, Stefan, Susanna LIEBER, Frank SCHAPER, Armin GEYER, Hans-Herbert BRINTZINGER, 2001. Anion exchange in alkyl-zirconocene borate ion pairs : are solvated alkyl-zirconocene cations relevant intermediates?. In: Journal of the American Chemical Society. 2001, 123(7), pp. 1483-1489. ISSN 0002-7863. eISSN 1520-5126. Available under: doi: 10.1021/ja003531wBibTex
@article{Beck2001Anion-23733,
year={2001},
doi={10.1021/ja003531w},
title={Anion exchange in alkyl-zirconocene borate ion pairs : are solvated alkyl-zirconocene cations relevant intermediates?},
number={7},
volume={123},
issn={0002-7863},
journal={Journal of the American Chemical Society},
pages={1483--1489},
author={Beck, Stefan and Lieber, Susanna and Schaper, Frank and Geyer, Armin and Brintzinger, Hans-Herbert}
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<dcterms:title>Anion exchange in alkyl-zirconocene borate ion pairs : are solvated alkyl-zirconocene cations relevant intermediates?</dcterms:title>
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<dcterms:abstract xml:lang="eng">Ion pairs of the type Cp<sup>x</sup><sub>2</sub>ZrMe<sup>+</sup>***A<sup>-</sup> containing various ansa-zirconocene methyl cations in contact with Me-B(C<sub>6</sub>F<sub>5</sub>)<sub>3</sub><sup>-</sup> or B(C<sub>6</sub>F<sub>5</sub>)<sub>4</sub><sup>-</sup> anions have been studied with regard to their anion exchange kinetics by 2D-NMR methods in benzene or toluene solutions. The resultsacceleration of anion exchange by added Li<sup>+</sup>***Me−B(C<sub>6</sub>F<sub>5</sub>)<sub>3</sub><sup>-</sup>, substantial nonproductive exchange between added and Zr-bound Me-B(C<sub>6</sub>F<sub>5</sub>)<sub>3</sub><sup>-</sup> anions, an increase of exchange rates at increased zirconocene concentrations, and the exclusively entropic origin of this rate increaseall indicate that anion exchange occurs by way of ion quadruples or higher ionic aggregates, rather than via dissociation to solvent-separated ions. These findings imply that solvent-separated (i.e. anion-free) alkyl zirconocene cations are unlikely to be relevant intermediates in reaction systems containing Cp<sup>x</sup><sub>2</sub>ZrMe<sup>+</sup>***A<sup>-</sup> ion pairs and, hence, also in zirconocene-based catalyst systems for the polymerization of α-olefins.</dcterms:abstract>
<dc:creator>Schaper, Frank</dc:creator>
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