期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 21, 期 16, 页码 6115-6122出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201406334
关键词
aluminium; density functional calculations; sustainable chemistry; polymers; ring-opening
资金
- ICIQ
- ICREA
- Spanish Ministerio de Economia y Competitividad (MINECO) [CTQ-2011-27385, CTQ2011-29054-C02-02]
- Severo Ochoa Excellence Accreditation [SEV-2013-0319]
- FPI fellowships
- AGAUR [2014-SGR-409]
- ICREA Funding Source: Custom
Amino-triphenolate derived Al-III complexes combined with suitable nucleophiles have been investigated as binary catalysts for the coupling of limonene oxide and carbon dioxide to afford alternating polycarbonates. These catalysts are able to produce stereoregular, perfectly alternating trans-polymers from cis-limonene oxide, whereas the pure trans isomer and cis/trans mixture give rise to lower degrees of stereoregularity. The best Al-III catalyst shows the potential to mediate the conversion of both stereoisomers of limonene oxide with high conversion levels of up to 71% under neat conditions, indicating the high degree of robustness and atom-efficiency of this catalytic process. Computational studies have revealed unique features of the binary catalyst system, among which is the preferred nucleophilic attack on the quaternary carbon centre in the limonene oxide substrate.
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