The Dual-Stereocontrol Mechanism: Heteroselective Polymerization of rac-Lactide and Syndioselective Polymerization of meso-Lactide by Chiral Aluminum Salan Catalysts.

aluminum poly(lactic acid) stereoregularity stereoselective polymerization syndiotactic polymer

Journal

Angewandte Chemie (International ed. in English)
ISSN: 1521-3773
Titre abrégé: Angew Chem Int Ed Engl
Pays: Germany
ID NLM: 0370543

Informations de publication

Date de publication:
07 10 2019
Historique:
received: 02 06 2019
pubmed: 30 7 2019
medline: 30 7 2019
entrez: 30 7 2019
Statut: ppublish

Résumé

We describe alkoxo-aluminum catalysts of chiral bipyrrolidine-based salan ligands that follow the dual-stereocontrol mechanism wherein a given combination of stereogeneities at the metal site and the proximal center of the last inserted lactidyl ("match") is active towards lactide having a proximal stereogenic center of the opposite configuration, while the diastereomeric combination of stereogeneities ("mismatch") is inactive towards any lactide. Polymerization of rac-LA by the enantiomerically pure catalysts was sluggish and gave stereoirregular poly(lactic acid) (PLA) because selective insertion to a match diastereomer gives a mismatch diastereomer. The racemic catalysts showed higher activity and led to highly heterotactic PLA following polymeryl exchange between two mismatched catalyst enantiomers. A succession of match diastereomers in selective meso-LA insertions led to syndiotactic PLAs reaching a syndiotacticity degree of α=0.96. This polymer featured a T

Identifiants

pubmed: 31355508
doi: 10.1002/anie.201906848
doi:

Types de publication

Journal Article Review Research Support, Non-U.S. Gov't

Langues

eng

Sous-ensembles de citation

IM

Pagination

14679-14685

Subventions

Organisme : Israel Science Foundation
ID : 553/18
Pays : International
Organisme : Israel Science Foundation and the University Grant Commission of India
ID : 2711/17
Pays : International
Organisme : MIUR-PRIN
ID : 2015CTEBBA
Pays : International
Organisme : POR FESR
ID : 2014/2010
Pays : International

Informations de copyright

© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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Auteurs

Rami Hador (R)

School of Chemistry, Tel Aviv University, Ramat Aviv, Tel Aviv, 6997801, Israel.

Antonio Botta (A)

Department of Chemistry and Biology A. Zambelli, and, INSTM Research Unit, University of Salerno, Fisciano, 84084 Salerno, Italy.

Vincenzo Venditto (V)

Department of Chemistry and Biology A. Zambelli, and, INSTM Research Unit, University of Salerno, Fisciano, 84084 Salerno, Italy.

Sophia Lipstman (S)

School of Chemistry, Tel Aviv University, Ramat Aviv, Tel Aviv, 6997801, Israel.

Israel Goldberg (I)

School of Chemistry, Tel Aviv University, Ramat Aviv, Tel Aviv, 6997801, Israel.

Moshe Kol (M)

School of Chemistry, Tel Aviv University, Ramat Aviv, Tel Aviv, 6997801, Israel.

Classifications MeSH