Department of Agricultural & Biological Engineering, University of Florida, PO Box 110570, Gainesville, FL 32611-0570, United States.
Department of Agricultural & Biological Engineering, University of Florida, PO Box 110570, Gainesville, FL 32611-0570, United States; Ministry of Forestry Bioethanol Research Center, Central South University of Forestry and Technology, Changsha, Hunan, 410004, China.
Carbohydr Polym. 2019 Dec 1;225:115207. doi: 10.1016/j.carbpol.2019.115207. Epub 2019 Aug 17.
Cellulose-based biocompatible, tunable and injectable hydrogels embedded with pH-responsive diblock copolymer micelles were constructed to achieve localized drug delivery with prolonged, stimuli-driven and slow-release function. First, we prepared two types of modified carboxymethyl cellulose (CMC) including hydrazide-modified carboxymethyl cellulose (CMC-NH) and oxidized carboxymethyl cellulose (CMC-CHO) with varying degrees of oxidation. Then, pH-responsive poly (ethylene oxide)-block-poly (2-(diisopropylamino) ethyl methacrylate) (PEO-b-PDPA) copolymers as micelle cores to carry hydrophobic substances were also synthesized through atom transfer radical polymerization (ATRP). An injectable hydrogel composite system was finally obtained by mixing CMC-NH and CMC-CHO polymer suspensions containing PEO-b-PDPA copolymer micelles through a Schiff base reaction. This newly-synthesized, tunable, cellulose-based double barrier system exhibits a pH-triggered, prolonged, and slow-release profile based on the release test using both Nile Red dye and doxorubicin. The hydrogel system also exhibited comparable storage moduli and tunable degradation properties.
构建了一种基于纤维素的生物相容性、可调且可注射的水凝胶,其中嵌入了对 pH 响应的两亲性嵌段共聚物胶束,以实现具有延长、刺激驱动和缓慢释放功能的局部药物输送。首先,我们制备了两种类型的改性羧甲基纤维素(CMC),包括带有不同氧化程度的腙改性羧甲基纤维素(CMC-NH)和氧化羧甲基纤维素(CMC-CHO)。然后,通过原子转移自由基聚合(ATRP)合成了作为载药胶束核的 pH 响应性聚(氧化乙烯)-嵌-聚(2-(二异丙基氨基)乙基甲基丙烯酸酯)(PEO-b-PDPA)共聚物。最后,通过席夫碱反应将含有 PEO-b-PDPA 共聚物胶束的 CMC-NH 和 CMC-CHO 聚合物悬浮液混合,得到可注射水凝胶复合材料体系。基于尼罗红染料和阿霉素的释放测试,新合成的、可调的、基于纤维素的双屏障系统表现出 pH 触发的、延长的、缓慢释放特性。水凝胶系统还表现出相当的储能模量和可调的降解性能。