期刊
POLYMER CHEMISTRY
卷 12, 期 23, 页码 3461-3470出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1py00288k
关键词
-
资金
- Natural Science Foundation of China [22073083, 21674095]
End-functionalization of oligomers with multiple H-bonding units is a feasible method to prepare supramolecular polymers. Competitive crystallization of H-bonding units and oligomeric blocks can drive supramolecular polymers to form long-range ordered structures. Thymine-monofunctionalized supramolecular poly(l-lactide) exhibits double-crystalline nature and controlled crystallization kinetics, providing insights into multi-step crystallization and crystallization-induced structural organization of semicrystalline supramolecular polymers.
End-functionalization of oligomers with multiple H-bonding units is a feasible method to prepare supramolecular polymers. Competitive crystallization of H-bonding units and oligomeric blocks can drive supramolecular polymers to form long-range ordered structures. Herein, we report the controlled synthesis, competitive crystallization kinetics, and crystallization-driven structural organization of thymine-monofunctionalized supramolecular poly(l-lactide) (PLLA-Thy). PLLA-Thy having a well-defined end-functionality and controlled molecular weight was synthesized by ring-opening polymerization using hydroxyl-functionalized thymine as the initiator. PLLA-Thy exhibits the double-crystalline nature, in which the PLLA block and the thymine terminal have a similar crystallization temperature (T-c) and melting point (T-m). The crystallizability of the thymine unit was depressed in PLLA-Thy with a long PLLA block. The thymine terminal and PLLA block revealed the competitive and coincident crystallization kinetics in PLLA-Thy with a medium thymine fraction, depending on T-c. Prompt crystallization of the thymine unit drove the lamellar organization of PLLA-Thy in a long range; the subsequent crystallization of the PLLA block segregated between thymine layers depressed the regularity of the lamellar ordering of PLLA-Thy. This work provides important insights into the multi-step crystallization and crystallization-induced structural organization of semicrystalline supramolecular polymers.
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