期刊
BIOMACROMOLECULES
卷 22, 期 2, 页码 640-648出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.biomac.0c01474
关键词
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资金
- European Regional Development Fund
- Estonian Research Council [MOBTT21, ResTA7, PRG339]
- Estonia-Russia Cross Border Cooperation Program [ER30]
- Baltic Research Program in Estonia (EEA grant) [EMP426]
- Swedish Research Council Formas [2016-00468]
- Swedish Foundation for Strategic Environmental Research through the STEPS project [2016/1489]
- Vinnova [2016-00468] Funding Source: Vinnova
- Formas [2016-00468] Funding Source: Formas
The study demonstrates that the properties of PAIMAs can be readily tuned by controlling the phase structure and transitions through the alkanoyl chain length and regiochemistry. Samples with different carbon chain lengths exhibit different properties, forming fully amorphous, semicrystalline, or liquid crystalline materials.
We have prepared a series of 12 D-isosorbide-2-alkanoate-5-methacrylate monomers as single regioisomers with different pendant linear C2-C20 alkanoyl chains using biocatalytic and chemical acylations. By conventional radical polymerization, these monomers provided high-molecular-weight biobased poly(alkanoyl isosorbide methacrylate)s (PAIMAs). Samples with C2-C12 alkanoyl chains were amorphous with glass transition temperatures from 107 to 54 degrees C, while C14-C20 chains provided semicrystalline materials with melting points up to 59 degrees C. Moreover, PAIMAs with C13-C20 chains formed liquid crystalline mesophases with transition temperatures up to 93 degrees C. The mesophases were studied using polarized optical microscopy, and rheology showed stepwise changes of the viscosity at the transition temperature. Unexpectedly, a PAIMA prepared from a regioisomeric monomer (C18) showed semicrystallinity but not liquid crystallinity. Consequently, the properties of the PAIMAs were readily tunable by controlling the phase structure and transitions through the alkanoyl chain length and the regiochemistry to form fully amorphous, semicrystalline, or semi/liquid crystalline materials.
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