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pH-Responsive supramolecular hydrogels for codelivery of hydrophobic and hydrophilic anticancer drugs

机译：pH响应超分子水凝胶可用于疏水和亲水抗癌药物的代码传递

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Codelivery of multiple drugs with one kind of drug carrier provides a promising strategy to suppress the drug resistance and achieve the enhanced therapeutic effect in cancer treatment. In this work, we successfully developed multifunctional supramolecular hydrogels based on in situ host-guest inclusion between polymer-drug conjugates and alpha-cyclodextrin to codeliver hydrophobic and hydrophilic anticancer drugs with pH-trigged release properties. Taking advantage of the strong hydrophobicity of 4 beta-aminopodophyllotoxin (NPOD), a derivative of podophyllotoxin (POD), the NPOD molecule was conjugated to low-molecular-weight methoxypoly (ethylene glycol) (mPEG) chain via a pH-responsive imine bond, forming an amphiphilic polymer-drug conjugates (NPOD-PEG). After adding alpha-cyclodextrin (alpha-CD) into the NPOD-PEG solutions, the stable supramolecular hydrogels were formed based on a combination of the partial inclusion complexation between one end of the mPEG blocks and alpha-CD and the hydrophobic aggregation of NPOD groups. The formed hydrogels could further efficiently load another hydrophilic anticancer drug doxorubicin (DOX) for combination therapy purposes. The hydrogel demonstrated unique gel-sol transition properties and pH-dependent dual drug release behavior due to the hydrolysis of imine bond at acidic environments. Furthermore, the cytotoxicity results suggested that the DOX loaded NPOD-PEG/alpha-CD hydrogels showed an enhanced cytotoxicity in cancer cells in comparison with single modality treatment and the resulting hydrogels are characterized by producing an additive cytotoxicity to cancer cells. In fact, the codelivery of two anticancer drugs with different physicochemical properties and anticancer mechanisms was a key to opening the door to their controlled drug delivery and enhanced anticancer effect. Therefore, DOX loaded NPOD-PEG/alpha-CD hydrogels as pH-trigged drug codelivery systems might have important potential for combination cancer chemotherapy.
机译：多种药物与一种药物载体的共递送为抑制耐药性并在癌症治疗中实现增强的治疗效果提供了一种有前途的策略。在这项工作中，我们成功地开发了基于聚合物-药物缀合物与α-环糊精之间原位客体包涵体的多功能超分子水凝胶，以共编码具有pH触发释放特性的疏水性和亲水性抗癌药物。利用鬼臼毒素（POD）衍生物4β-氨基鬼臼毒素（NPOD）的强疏水性，该NPOD分子通过pH响应亚胺键与低分子量甲氧基聚（乙二醇）（mPEG）链结合。 ，形成两亲性聚合物-药物偶联物（NPOD-PEG）。将α-环糊精（α-CD）添加到NPOD-PEG溶液中后，基于mPEG嵌段和α-CD的一端之间的部分包合络合和NPOD基团的疏水性聚集的结合，形成了稳定的超分子水凝胶。 。形成的水凝胶可进一步有效地负载另一种亲水性抗癌药物阿霉素（DOX），以用于联合治疗。由于在酸性环境下亚胺键的水解，水凝胶显示出独特的凝胶-溶胶转变特性和依赖pH的双重药物释放行为。此外，细胞毒性结果表明，与单模治疗相比，载有DOX的NPOD-PEG /α-CD水凝胶在癌细胞中显示出增强的细胞毒性，并且所得水凝胶的特征在于对癌细胞产生附加的细胞毒性。实际上，两种具有不同理化性质和抗癌机制的抗癌药物的代码传递是打开控制其药物传递和增强抗癌作用之门的关键。因此，作为pH触发的药物代码传递系统，载有DOX的NPOD-PEG /α-CD水凝胶可能具有联合癌症化疗的重要潜力。

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