Serially pH-Modulated Hydrogels Based on Boronate Ester and Polydopamine Linkages for Local Cancer Therapy,ACS Applied Materials & Interfaces

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Serially pH-Modulated Hydrogels Based on Boronate Ester and Polydopamine Linkages for Local Cancer Therapy
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-01-08 , DOI: 10.1021/acsami.0c16199
Song Yi Lee _{1,

2} , Mingyu Yang ₁ , Ji-Hye Seo ₁ , Da In Jeong ₁ , ChaeRim Hwang ₁ , Han-Jun Kim _{3,

4,

5} , Junmin Lee _{3,

4,

5} , KangJu Lee _{3,

4,

5} , JiHye Park ₁ , Hyun-Jong Cho _{1,

2}

Affiliation

Elaborately and serially pH-modulated hydrogels possessing optimized viscoelastic natures for short gelation time and single syringe injection were designed for peritumoral injection of an anticancer agent. Boronate ester bonds between phenylboronic acid (PBA) (installed in HA-PBA (HP)) and dopamine (included in HA-dopamine (HD)) along with self-polymerization of dopamine (via interactions between HD conjugates) were introduced as the main cross-linking strategies of a hyaluronic acid (HA) hydrogel. Considering pK_a values (8.0–9.5) of PBA and dopamine, the pH of each polymer dispersion was controlled elaborately for injection through a single syringe, and the final pH was tuned nearby the physiological pH (pH 7.8). The shear-thinning behavior, self-healing property, and single syringe injectability of a designed hydrogel cross-linked nearby physiological pH may provide its convenient application to peritumoral injection and prolonged retention in local cancer therapy. Erlotinib (ERT) was encapsulated in a microsphere (MS), and it was further embedded in an HP/HD-based hydrogel for sustained and locoregional delivery. A rheologically tuned hydrogel containing an ERT MS exhibited superior tumor-suppressive efficiencies compared to the other groups in A549 tumor-bearing mice. A designed injectable hydrogel through a single syringe system may be efficiently applied to local cancer therapy with lower toxicities to healthy organs.

中文翻译：

基于硼酸酯和聚多巴胺连接的系列pH调节水凝胶用于局部癌症治疗

精心设计和连续调节pH值的水凝胶，具有优化的粘弹性，可缩短胶凝时间，并设计单针筒注射用于肿瘤周围注射抗癌剂。主要介绍了苯基硼酸（PBA）（安装在HA-PBA（HP）中）和多巴胺（包括在HA-多巴胺（HD）中）之间的硼酸酯键以及多巴胺的自聚合（通过HD共轭物之间的相互作用）透明质酸（HA）水凝胶的交联策略。考虑p K _a如果将PBA和多巴胺的值（8.0-9.5）调节到适当水平，则可以通过单个注射器对每种聚合物分散体的pH进行精细控制，并在生理pH（pH 7.8）附近调整最终pH。设计的水凝胶交联的附近生理pH值的剪切稀化行为，自我修复性能和单针筒可注射性可为其在肿瘤周围注射中的便捷应用和在局部癌症治疗中的长期保留提供便利。厄洛替尼（ERT）被封装在微球（MS）中，并进一步嵌入基于HP / HD的水凝胶中，以实现持续和局部区域递送。与A549荷瘤小鼠中的其他组相比，含有ERT MS的流变调谐水凝胶显示出优异的抑瘤效率。

更新日期：2021-01-20

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