Data_Sheet_1_Fabrication of Customized Nanogel Carriers From a UV-Triggered Dynamic Self-Assembly Strategy.PDF

Recent advances in self-assembled nanogel carriers have allowed precise design of hierarchical structures by a low-cost solution-phase approach. Typically, photochemical strategy on the tailor of morphology and dimension has emerged as a powerful tool, because light-trigger has exceptional advantages of an instant “on/off” function and spatiotemporal precision at arbitrary time. Herein, we report a tunable manipulation of sequentially morphological transition via a “living” thiol-disulfide exchange reaction from a UV-tailored hierarchical self-assembly strategy. By varying the irradiation time, the photochemical method can easily fabricate and guide a series of attractively architectural evolution in dilute aqueous solutions, by which the improving hydrophobicity and sensitive redox-responsiveness endowed these disulfide-linked nanoparticles with remarkable capacities of abundant encapsulation, effective separation, and controlled release of hydrophobic cargoes. Notably, once the exchange reaction is suspended at any point of time by removing the UV lamp, these active sites within the nanogel carriers are instantaneous deactivated and the correspondingly structural transformations are also not conducted any more. However, if the stable inert sites are reactivated as needed by turning on the UV light, the interrupting morphology evolution can continue its previous steps, which may provide a simple and novel approach to fabricating the desired self-assemblies in solutions. With regard to this advanced functionality, various nanogel carriers with customizable structures and properties have been yielded and screened for cancer therapy. Thus, this “living” controlled self-assembled method to program morphology evolution in situ is a universal strategy that will pave novel pathways for creating sequential shape-shifting and size-growing nanostructures and constructing uniform nanoscopic functional entities for advanced bio-applications.

近年来，自组装纳米凝胶载体的研究取得了显著进展，通过低成本溶液相方法实现了对分级结构的精确设计。通常，在形态和尺寸的定制方面，光化学策略已成为一种强大的工具，这是因为光触发的“开/关”功能具有瞬间响应的优势，以及任意时间点的时空精确性。在本研究中，我们报道了一种通过“活”硫醇-二硫键交换反应对顺序形态转变进行可调操控的方法，该方法基于紫外定制分级自组装策略。通过调节辐照时间，光化学方法可以轻松地在稀水溶液中制造并引导一系列引人入胜的建筑性演化，从而赋予这些二硫键连接的纳米颗粒改善的疏水性和敏感的氧化还原响应性，使其在疏水性药物的包封、有效分离和可控释放方面展现出显著的能力。值得注意的是，一旦通过移除紫外灯在任何时间点暂停交换反应，纳米凝胶载体中的活性位点将立即失活，相应的结构转变也将停止。然而，当通过开启紫外灯重新激活所需的稳定惰性位点时，中断的形态演化可以继续其之前的步骤，这或许为在溶液中制造所需的自我组装提供了一种简单而新颖的方法。鉴于这种高级功能，各种具有可定制结构和特性的纳米凝胶载体已被制备并筛选用于癌症治疗。因此，这种在原位编程形态演化的“活”可控自组装方法是一种通用的策略，将为创建连续形状变换和尺寸增长纳米结构以及构建用于高级生物应用的均匀纳米级功能实体开辟新的途径。