Narrowly Dispersed, Degradable, and Scalable Poly(oligoethylene glycol methacrylate)-Based Nanogels via Thermal Self-Assembly,Industrial & Engineering Chemistry Research

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Narrowly Dispersed, Degradable, and Scalable Poly(oligoethylene glycol methacrylate)-Based Nanogels via Thermal Self-Assembly
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2018-05-25 , DOI: 10.1021/acs.iecr.8b00793
Madeline J. Simpson ₁ , Brandon Corbett ₁ , Ana Arezina ₁ , Todd Hoare ₁

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Covalently cross-linked and hydrolytically degradable poly(oligoethylene glycol methacrylate) (POEGMA)-based nanogels are fabricated using an all-aqueous self-assembly approach. The nanogels are composed of hydrazide- (POH) and aldehyde-functionalized (POA) POEGMA precursor polymers that exhibit lower critical solution temperature (LCST) behavior in aqueous media and form a covalent, yet degradable, hydrazone linkage upon mixing. By systematically changing the chemistry of the core and cross-linking precursor polymers, the concentration of the core precursor polymer, the ratio of core to cross-linking precursor polymer, and the temperature at which the assembly is conducted, a library of nanogels was produced with significant differences in size, polydispersity, and colloidal stability. Multivariate statistics indicates the presence of significant nonlinear responses within the process variables as well as correlations between the output variables, reflective of the complex balance of aggregation and stabilization mechanisms at play to produce a stable, monodisperse nanogel population. Furthermore, formulations that yield more polydisperse nanogels on a small scale result in macroscopic aggregate formation when scaled up while formulations that yield more monodisperse nanogels can be scaled to yield nanogels with matched properties. We anticipate these results can be applied to strategically synthesize stable, covalently cross-linked, degradable nanogels with targeted sizes at scalable quantities for a range of biomedical and biosensing applications.

中文翻译：

通过热自组装的窄分散，可降解和可扩展的聚（低聚乙二醇甲基丙烯酸甲酯）纳米凝胶

共价交联和可水解降解的聚（甲基丙烯酸低聚乙二醇酯）（POEGMA）基纳米凝胶是使用全水自组装方法制备的。纳米凝胶由酰肼（POH）和醛官能化（POA）POEGMA前体聚合物组成，它们在水性介质中的临界溶液温度（LCST）行为较低，并且在混合时形成共价但可降解的键。通过系统地改变核心和交联前体聚合物的化学性质，核心前体聚合物的浓度，核心与交联前体聚合物的比例以及进行组装的温度，产生了纳米凝胶库在尺寸，多分散性和胶体稳定性方面存在显着差异。多变量统计数据表明过程变量中存在显着的非线性响应，以及输出变量之间的相关性，反映了聚集的稳定平衡和稳定机制在产生稳定的单分散纳米凝胶种群方面的作用。此外，小规模生产更多多分散纳米凝胶的制剂在按比例放大时会导致宏观聚集体的形成，而单产更多单分散纳米凝胶的制剂可以按比例缩放以产生具有匹配特性的纳米凝胶。我们预期这些结果可用于战略性地合成稳定，共价交联的可降解纳米凝胶，其目标尺寸可缩放的量适用于一系列生物医学和生物传感应用。

更新日期：2018-05-27

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