通过活性聚合诱导结晶驱动的自组装，具有聚碳酸酯芯的可扩展且均匀长度可调的生物可降解嵌段共聚物纳米纤维,Journal of the American Chemical Society

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通过活性聚合诱导结晶驱动的自组装，具有聚碳酸酯芯的可扩展且均匀长度可调的生物可降解嵌段共聚物纳米纤维
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-10-28 , DOI: 10.1021/jacs.2c09715
Charlotte E Ellis ₁ , J Diego Garcia-Hernandez ₁ , Ian Manners _{1,

2}

Affiliation

通过称为活结晶驱动自组装 (CDSA) 的种子生长方法制备的均匀一维嵌段共聚物 (BCP) 纳米纤维由于其各向异性、长度可调性和可变的核心和日冕化学性质，为各种应用提供了有希望的潜力。然而，此过程由涉及独立 BCP 合成和自组装步骤的多步骤过程组成，其中后者在低溶液浓度（<1 wt%）下进行，阻碍了放大。在这里，我们展示了使用一锅法 BCP 合成和自组装过程、聚合诱导 CDSA (PI-CDSA) 来获得具有可生物降解结晶聚（氟代亚甲基碳酸酯）（PFTMC）核和亲水性的长度分散纳米纤维。源自 PEG- b的聚乙二醇 (PEG) 冠-浓度高达 20 wt% 的 PFTMC，比之前报道的浓度高 400 倍。此外，活性 PI-CDSA 可用于获取浓度高达 10 wt% 的可扩展、低分散性和长度可调的 1D PEG- b -PFTMC 纳米纤维。这提供了第一个涉及全有机和可生物降解 BCP 的活性 PI-CDSA 示例，该 BCP 使用方便实施的 BCP 合成协议，并且不涉及活性阴离子聚合。值得注意的是，控制长度从 100 到 660 nm ( L _w / L _n= 1.08–1.20) 的制备，允许在有用的长度尺度上扩大获得明确定义的可生物降解纳米纤维，以用于纳米医学应用。有趣的是，详细研究揭示了 PFTMC 均聚物杂质在所用反应条件下原位制备的 BCP 中纳米纤维形成过程中的关键作用。

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Scalable and Uniform Length-Tunable Biodegradable Block Copolymer Nanofibers with a Polycarbonate Core via Living Polymerization-Induced Crystallization-Driven Self-assembly

Uniform 1D block copolymer (BCP) nanofibers prepared by the seeded-growth approach termed living crystallization-driven self-assembly (CDSA) offer promising potential for various applications due to their anisotropy, length tunability, and variable core and coronal chemistries. However, this procedure consists of a multi-step process involving independent BCP synthesis and self-assembly steps, where the latter is performed at low solution concentrations (<1 wt %), hindering scale-up. Here, we demonstrate the use of a one-pot BCP synthesis and self-assembly process, polymerization-induced CDSA (PI-CDSA), to access length-disperse nanofibers with a biodegradable crystalline poly(fluorenetrimethylenecarbonate) (PFTMC) core and a hydrophilic poly(ethylene glycol) (PEG) corona derived from PEG-b-PFTMC at concentrations up to 20 wt %, 400 times higher than those previously reported. Furthermore, living PI-CDSA could be used to access scalable, low dispersity, and length-tunable 1D PEG-b-PFTMC nanofibers at concentrations of up to 10 wt %. This provides the first example of living PI-CDSA involving an all-organic and biodegradable BCP that utilizes a conveniently implemented BCP synthesis protocol and does not involve living anionic polymerization. Significantly, samples of low-dispersity nanofibers of controlled lengths from 100 to 660 nm (L_w/L_n = 1.08–1.20) were prepared, allowing for upscaled access to well-defined biodegradable nanofibers at useful length-scales for applications in nanomedicine. Interestingly, detailed studies revealed a key role for PFTMC homopolymer impurities in the BCP prepared in situ in the formation of nanofibers under the reaction conditions used.

更新日期：2022-10-28

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