Precise Control of Two-Dimensional Platelet Micelles from Biodegradable Poly(p-dioxanone) Block Copolymers by Crystallization-Driven Self-Assembly,Macromolecules

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Precise Control of Two-Dimensional Platelet Micelles from Biodegradable Poly(p-dioxanone) Block Copolymers by Crystallization-Driven Self-Assembly
Macromolecules ( IF 5.1 ) Pub Date : 2022-09-06 , DOI: 10.1021/acs.macromol.2c01158
Xu Zhang ₁ , Guanhao Chen ₁ , Liping Liu ₁ , Lingyuan Zhu ₁ , Zaizai Tong ₁

Affiliation

Two-dimensional (2D) core–shell nanoparticles have been attracting increasing interest due to their wide applications in materials science. Living crystallization-driven self-assembly (CDSA) is an ambient temperature, seeded growth method of crystallizable block copolymers (BCPs) in selective solvents, which has been demonstrated to be a powerful tool for the creation of one-dimensional (1D)/2D nanomaterials with precise control over size and compositions. Nevertheless, the development of an efficient living CDSA approach is a challenge for the case of semicrystalline poly(p-dioxanone) (PPDO) as a core-forming block, where the dimensional control is poor. Herein, we demonstrate that the insufficient size control of 2D PPDO platelets could be overcome through modulation of solvent compositions or elevating the crystallization temperatures for PPDO. The possible mechanism involves an improved unimer solubility that avoids fast unimer aggregation. As a result, uniform 2D platelet micelles with a controlled area over a substantial size range are created via epitaxial growth of the unimer. It is noteworthy that the shape control of 2D platelet micelles from quasi-square to elongated hexagon to lozenge shapes can be accessible by regulating the crystallization conditions such as adding different amounts of cosolvents or crystallization at an elevated temperature. Meanwhile, spatially defined block comicelles can be achieved via the seeded growth approach from PPDO core-forming BCPs with different corona functionalities at elevated temperatures. The excellent water stability and biocompatibility properties of 2D PPDO platelet micelles further enable them to have a potential application as cargo vehicles in the drug delivery field.

中文翻译：

通过结晶驱动自组装精确控制可生物降解聚 (p-二恶烷酮) 嵌段共聚物的二维血小板胶束

二维（2D）核壳纳米粒子由于其在材料科学中的广泛应用而受到越来越多的关注。活性结晶驱动自组装 (CDSA) 是一种环境温度、可结晶嵌段共聚物 (BCP) 在选择性溶剂中的晶种生长方法，已被证明是创建一维 (1D)/2D 的有力工具可以精确控制尺寸和成分的纳米材料。然而，对于半结晶多晶硅（p-二恶烷酮）（PPDO）作为成芯块，其中尺寸控制很差。在这里，我们证明了可以通过调节溶剂成分或提高 PPDO 的结晶温度来克服二维 PPDO 片晶尺寸控制不足的问题。可能的机制涉及避免快速单聚体聚集的改进的单聚体溶解度。结果，通过单聚体的外延生长，产生了在相当大的尺寸范围内具有受控面积的均匀二维血小板胶束。值得注意的是，通过调节结晶条件（例如添加不同量的助溶剂或在升高的温度下结晶），可以实现从准正方形到细长六边形到菱形的二维片状胶束的形状控制。同时，可以通过在高温下具有不同电晕功能的 PPDO 核心形成 BCP 的种子生长方法来实现空间定义的块状相框。二维 PPDO 血小板胶束优异的水稳定性和生物相容性进一步使它们在药物输送领域具有作为货运载体的潜在应用。

更新日期：2022-09-06

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