期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 29, 页码 9797-9801出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201902833
关键词
Lewis pairs; Michael-type monomers; neutron diffraction; polymerization; X-ray diffraction
资金
- Studienstiftung d. dt. Volkes
- FCI scholarship
- TUM GS
- LRZ of the Bavarian Academy of Science
Deprotonation usually occurs as an unwanted side reaction in the Lewis pair polymerization of Michael acceptors, for which the conjugated addition of the Lewis base to the acidactivated monomer is the commonly accepted initiation mechanism. This has also been reported for B-P-based bridged Lewis pairs (BLPs) that form macrocyclic addition products. We now show that the formerly unwanted deprotonation is the likely initiation pathway in the case of Al-P-based BLPs. In a detailed study of a series of Al-P-based BLPs, using a combination of single-crystal diffraction experiments (X-ray and neutron) and mechanistic investigations (experimental and computational), an active role of the methylene bridge was revealed, acting as a base towards the a-acidic monomers. Additionally, the polymerization studies proved a living behavior combined with significantly high activities, narrow molecular mass distributions, and the possibility of copolymerization.
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