Centre for Advanced Macromolecular Design and Australian Centre for NanoMedicine, School of Chemical Engineering, The University of New South Wales, Sydney, NSW, 2052, Australia.
Electron Microscope Unit, Mark Wainwright Analytical Centre, The University of New South Wales, Sydney, NSW, 2052, Australia.
Macromol Rapid Commun. 2020 Jan;41(1):e1900493. doi: 10.1002/marc.201900493. Epub 2019 Nov 10.
In this work, the authors report a novel single-step, one-pot process for the synthesis of self-assembled nanoparticles using a polymerization-induced self-assembly (PISA) mechanism. In contrast to conventional approaches employing a pre-formed macromolecular stabilizer, the disparate reactivities between two monomers, oligo(ethylene glycol) methyl ether methacrylate (OEGMA) and diacetone acrylamide (DAAm), are exploited instead to synthesize a gradient copolymer directly in aqueous solution. Due to the hydrophobicity of poly(DAAm), these gradient copolymers can self-assemble in situ to form spheres and worms stabilized by the OEGMA residues. A surprisingly broad range of parameters are identified in which the worm morphology can be stabilized, which is highlighted by significant gelation of the reaction mixture in situ. This single-step gradient copolymerization approach to PISA is more efficient than conventional two-step syntheses. These results demonstrate improved reproducibility owing to the production of self-assembled nanoparticles directly in a one-pot and single-step synthesis.
在这项工作中，作者报告了一种使用聚合诱导自组装（PISA）机制合成自组装纳米粒子的新颖的单步、一锅法。与传统方法采用预先形成的大分子稳定剂不同，作者利用两种单体——聚乙二醇甲基醚甲基丙烯酸酯（OEGMA）和二丙酮丙烯酰胺（DAAm）之间的差异反应性，直接在水溶液中合成梯度共聚物。由于聚（DAAm）的疏水性，这些梯度共聚物可以在原位自组装形成由 OEGMA 残基稳定的球体和蠕虫。令人惊讶的是，确定了可以稳定蠕虫形态的广泛参数范围，这突出体现在反应混合物在原位显著胶凝。与传统的两步合成相比，这种一步梯度共聚的 PISA 方法更有效。这些结果表明，由于自组装纳米粒子直接在一锅和一步合成中生成，因此提高了重现性。
