We demonstrated a new methodology for the templated synthesis of a crosslinked poly(disulfide)s-based dynamic covalent nanonetwork as a highly stable potential delivery vehicle for chemotherapeutic applications. The synthesis was carried out by treatment of a nanoaggregate of a biomass-derived lipoic acid-based amphiphilic monomer with a reducing agent at room temperature in open air and aqueous medium. The hydrodynamic diameter of the naoaggregate was ∼130 nm as probed by dynamic light scattering. Control over the crosslinking density was achieved by varying the ratio of monomer : reducing agent. The crosslinking percentage varied from ∼13% to ∼100%. This provided the opportunity of fine-tuning the stability of the nanocarrier, noncovalent encapsulation stabilities and kinetics of cargo release, which are highly relevant in drug-delivery applications. For a highly crosslinked nanonetwork, in the simulated redox condition of cancer cells, ∼80% release of the guest molecule was noted from the nanonetwork in a sustained manner. Controlled depolymerization of the polymer was accomplished by use of specific mol% of the same reducing agent. Finally, the reversibility and recyclability of the poly(disulfide)s to the monomeric form was achieved by treatment of the polymer with an external thiol in the presence of an organic base.

中文翻译：

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动态共价聚（二硫键）纳米网络的还原剂触发模板合成：非共价封装稳定性和货物释放的显着调整


我们展示了一种基于交联聚（二硫键）s 的动态共价纳米网络的模板化合成新方法，作为化疗应用中高度稳定的潜在递送载体。通过在室温下在露天和水性介质中用还原剂处理生物质衍生的硫辛酸基两亲性单体的纳米聚集体进行合成。通过动态光散射探测 naoaggregate 的流体动力学直径为 ∼130 nm。通过改变单体：还原剂的比例来控制交联密度。交联百分比从 ∼13% 到 ∼100% 不等。这为微调纳米载体的稳定性、非共价包封稳定性和货物释放动力学提供了机会，这在药物递送应用中高度相关。对于高度交联的纳米网络，在癌细胞的模拟氧化还原条件下，以持续的方式从纳米网络中观察到 ∼80% 的客体分子释放。通过使用相同还原剂的特定 mol% 来完成聚合物的受控解聚。最后，通过在有机碱存在下用外部硫醇处理聚合物，实现了聚（二硫化物）对单体形式的可逆性和可回收性。