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Kinetic Self-Assembly of Hierarchical V-Notch Spherulites via Asynchronous Polymerization-Crystallization for
Shengli Chen1, Yiming Wang1, Xuelei Dong1
1Hebei Key Laboratory of Functional Polymers, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300401, P. R. China.
Journal of the American Chemical Society
|March 4, 2026
Summary
Researchers developed a new method for creating complex anisotropic spherulites using controlled polymerization and crystallization kinetics. This technique enables the engineering of materials with advanced anticounterfeiting properties.
Area of Science:
- Materials Science
- Polymer Chemistry
- Crystallization Science
Background:
- Controlled self-assembly of anisotropic spherulites is challenging due to thermodynamic preferences for isotropic structures.
- Transient crystallization intermediates complicate the formation of ordered anisotropic structures.
Purpose of the Study:
- To present a conceptual advance in polymerization-induced crystallization-driven self-assembly (PI-CDSA).
- To direct the formation of anisotropic spherulites by harnessing kinetic asynchrony between polymerization and crystallization.
Main Methods:
- Utilized a bulk PI-CDSA (BPI-CDSA) protocol at low temperature (10 °C).
- Leveraged steric hindrance and secondary crystallization under supercooling.
- Confirmed asynchronous kinetics using in situ solid-state NMR and wide-angle X-ray scattering.
Main Results:
- Achieved precise control over 3D hierarchical anisotropic spherulites with V-notch defects from poly(δ-valerolactone) (PVL).
- Revealed a nonequilibrium self-assembly pathway via metastable intermediates (nanorods, hedrites, dendritic sheaves, "two-eyed" spherulites).
- Demonstrated successful engineering of V-notch spherulites onto cellulose fibers for specialty paper with anticounterfeiting capabilities.
Conclusions:
- Established a kinetic-control paradigm for nonequilibrium self-assembly.
- Opened avenues for advanced materials through defect-guided engineering.
- Highlighted the potential of V-notch spherulites for functional applications like anticounterfeiting.
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