Tianjin Key Laboratory of Pulp and Paper, Tianjin University of Science & Technology, Tianjin 300457, China.
CAS Key Laboratory of Bio-Based Material, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China.
ACS Appl Mater Interfaces. 2020 Dec 23;12(51):57410-57420. doi: 10.1021/acsami.0c15465. Epub 2020 Dec 8.
The development of intelligent and multifunctional hydrogels having photothermal properties, good mechanical properties, sustained drug release abilities with low burst release, antibacterial properties, and biocompatibility is highly desirable in the biomaterial field. Herein, mesoporous polydopamine (MPDA) nanoparticles wrapped with graphene oxide (GO) were physically cross-linked in cellulose nanofibril (CNF) hydrogel to obtain a novel MPDA@GO/CNF composite hydrogel for controllable drug release. MPDA nanoparticles exhibited a high drug loading ratio (up to 35 wt %) for tetracycline hydrochloride (TH). GO was used to encapsulate MPDA nanoparticles for extending the drug release time and reinforcing the physical strength of the obtained hydrogel. The mechanical strength of the as-fabricated MPDA@GO/CNF composite hydrogel was five times greater compared to that of the pure CNF hydrogel. Drug release experiments demonstrated that burst release behavior was significantly reduced by adding MPDA@GO. The drug release time of the MPDA@GO/CNF composite hydrogel was 3 times and 7.2 times longer than that of the polydopamine/CNF hydrogel and pure CNF hydrogel, respectively. The sustained and controlled drug release behaviors of the composite hydrogel were highly dependent on the proportion of MPDA and GO. Moreover, the rate of drug release could be accelerated by near-infrared (NIR) light irradiation and pH value change. The drug release kinetics of the as-prepared composite hydrogel was well described by the Korsmeyer-Peppas model, and the drug release mechanism of TH from the composite hydrogel was anomalous transport. Importantly, this carefully designed MPDA@GO/CNF composite hydrogel showed good biocompatibility through an cytotoxicity test. In particular, the toxicity of GO was well shielded by the CNF hydrogel. Therefore, this novel MPDA@GO/CNF composite hydrogel with an encapsulation structure for controllable drug release and toxicity shielding of GO could be used as a very promising controlled drug delivery carrier, which may have potential applications for chemical and physical therapies.
具有光热性能、良好的机械性能、低突释持续药物释放能力、抗菌性能和生物相容性的智能多功能水凝胶的发展在生物材料领域是非常需要的。在此，介孔聚多巴胺（MPDA）纳米粒子被包裹在氧化石墨烯（GO）中，并在纤维素纳米纤维（CNF）水凝胶中物理交联，以获得一种用于可控药物释放的新型 MPDA@GO/CNF 复合水凝胶。MPDA 纳米粒子对盐酸四环素（TH）的载药率高达 35wt%。GO 被用来包裹 MPDA 纳米粒子，以延长药物释放时间并增强所得到的水凝胶的物理强度。与纯 CNF 水凝胶相比，所制备的 MPDA@GO/CNF 复合水凝胶的机械强度增加了五倍。药物释放实验表明，加入 MPDA@GO 后，突释行为显著减少。MPDA@GO/CNF 复合水凝胶的药物释放时间分别比聚多巴胺/CNF 水凝胶和纯 CNF 水凝胶延长了 3 倍和 7.2 倍。复合水凝胶的药物持续和控制释放行为高度依赖于 MPDA 和 GO 的比例。此外，近红外（NIR）光照射和 pH 值变化可以加速药物释放。所制备的复合水凝胶的药物释放动力学很好地符合 Korsmeyer-Peppas 模型，TH 从复合水凝胶中的药物释放机制为异常传输。重要的是，这种精心设计的 MPDA@GO/CNF 复合水凝胶通过细胞毒性试验显示出良好的生物相容性。特别是，GO 的毒性被 CNF 水凝胶很好地屏蔽了。因此，这种具有封装结构的新型 MPDA@GO/CNF 复合水凝胶具有可控药物释放和 GO 毒性屏蔽的功能，可用作一种很有前途的控制药物输送载体，可能在化学和物理治疗中有潜在应用。
