Initiated Chemical Vapor Deposition Kinetics of Poly(4-aminostyrene).
Initiated Chemical Vapor Deposition Kinetics of Poly(4-aminostyrene).
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DOI：
10.3389/fbioe.2021.670541
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发表时间：
2021
影响因子：
5.7
通讯作者：
Yang R
中科院分区：
文献类型：
--
作者：
Khlyustova A;Yang R
引发化学气相沉积（iCVD）是一种用于合成功能聚合物薄膜的自由基聚合技术。在药物递送的背景下，iCVD涂层的保形性和多种功能性化学部分使其成为用于封装药物的优异材料。聚（4-氨基苯乙烯）（PAS）属于一类可官能化的材料，其伯胺允许用生物分子修饰递送载体，从而实现靶向递送或生物相容性。了解iCVD中PAS聚合的动力学对于这种部署至关重要，因为薄膜封装中的药物释放动力学已被证明是由膜厚度决定的。然而，沉积条件对PAS生长动力学的影响尚未得到系统的研究。为了弥合这一知识差距，我们报告了iCVD聚合的动力学作为单体的分数饱和压力的函数（即，Pm/Psat），在低Pm/Psat下具有二次依赖性，在高Pm/Psat下具有线性依赖性。我们发现临界Pm/Psat值为0.2，在该值附近，许多其他iCVD单体也发生了转变。由于现有的iCVD过程的理论模型不能完全解释的双制度聚合动力学，我们从溶液相聚合的灵感，并提出了更新的终止机制，占两个制度之间的过渡。报告的模型建立在现有的iCVD理论，并允许PAS薄膜的合成与精确控制的生长速率，这有可能加速部署的iCVD PAS作为一种新型的生物材料在控制和靶向药物输送与设计的药代动力学。
Initiated Chemical Vapor Deposition (iCVD) is a free-radical polymerization technique used to synthesize functional polymer thin films. In the context of drug delivery, the conformality of iCVD coatings and the variety of functional chemical moieties make them excellent materials for encapsulating pharmaceutics. Poly(4-aminostyrene) (PAS) belongs to a class of functionalizable materials, whose primary amine allows decoration of the delivery vehicles with biomolecules that enable targeted delivery or biocompatibility. Understanding kinetics of PAS polymerization in iCVD is crucial for such deployments because drug release kinetics in thin-film encapsulation have been shown to be determined by the film thickness. Nevertheless, the effects of deposition conditions on PAS growth kinetics have not been studied systematically. To bridge that knowledge gap, we report the kinetics of iCVD polymerization as a function of fractional saturation pressure of the monomer (i.e., Pm/Psat) in a dual-regime fashion, with quadratic dependence under low Pm/Psat and linear dependence under high Pm/Psat. We uncovered the critical Pm/Psat value of 0.2, around which the transition also occurs for many other iCVD monomers. Because existing theoretical models for the iCVD process cannot fully explain the dual-regime polymerization kinetics, we drew inspiration from solution-phase polymerization and proposed updated termination mechanisms that account for the transition between two regimes. The reported model builds upon existing iCVD theories and allows the synthesis of PAS thin films with precisely controlled growth rates, which has the potential to accelerate the deployment of iCVD PAS as a novel biomaterial in controlled and targeted drug delivery with designed pharmacokinetics.
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