HAL Id: hal-00264971
https://hal.archives-ouvertes.fr/hal-00264971
Submitted on 18 Mar 2008
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“Half-lanthanidocenes catalysts via the
”borohydride/alkyl” route: A simple approach of ligand screening for the controlled polymerization of styrene.”
Philippe Zinck, Andreia Valente, Michael Terrier, André Mortreux, Marc Visseaux
To cite this version:
Philippe Zinck, Andreia Valente, Michael Terrier, André Mortreux, Marc Visseaux. “Half- lanthanidocenes catalysts via the ”borohydride/alkyl” route: A simple approach of ligand screening for the controlled polymerization of styrene.”. Comptes rendus de l’Académie des sciences. Série IIc, Chimie, Elsevier, 2008, sous presse. �10.1016/j.crci.2007.12.006�. �hal-00264971�
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