pH响应性木质素水凝胶的制备及药物控释  

Preparation of lignin-based pH responsive hydrogel and its application in controlled drug release

作　　者：于丁一 李圆圆 王晨钰 纪永升[1] YU Dingyi;LI Yuanyuan;WANG Chenyu;JI Yongsheng(College of Pharmacy,Henan University of Chinese Medicine,Zhengzhou 450046,Henan,China)

机构地区：[1]河南中医药大学药学院,河南郑州450046

出　　处：《化工进展》2023年第6期3138-3146,共9页Chemical Industry and Engineering Progress

基　　金：河南中医药大学高层次人才引进专项(00104311-2022-1-1-16);河南省高等学校重点科研项目(23A150033)。

摘　　要：以从松木提取的水溶性碱木质素(AL)为原料,利用3-氯-2-羟丙基三甲基氯化铵对AL进行季铵化改性,成功制备一种阴阳离子两性木质素(AML-45)。在8g/L NaOH、12g/L尿素和-10℃环境中对AML-45进行活化,活化后在碱性介质中与聚乙二醇二缩水甘油醚(PEGDGE)共聚合成制备木质素基pH响应性水凝胶。通过傅里叶红外光谱仪和激光粒度分析仪(DLS)等对AML-45和AML-45基水凝胶结构进行表征,利用扫描电子显微镜对木质素基水凝胶的形貌特征进行表征,研究该水凝胶在不同pH的PBS缓冲溶液中的溶胀行为。结果显示,水凝胶具有明显的pH响应性,在酸性范围内,当pH为4时溶胀率最低为260%,pH为7.4时最高可达到330%。此外,水凝胶的溶胀率与AML-45浓度、交联剂PEGDGE用量和反应环境pH有关。以5-氟尿嘧啶作为模型药物,探讨其在酸性范围内(pH=2~7.4)缓冲介质中药物释放行为。在30h内,负载药物后的水凝胶在缓冲溶液(pH=7.4)中的药物累积释放量可达78%,高于酸性缓冲环境(pH=4)的62%和(pH=2)69%药物累积释放量,故此水凝胶有明显的药物缓释作用。A water-soluble alkali lignin(AL)extracted from pine wood was used as raw material to prepared amphoteric lignin(AML-45)which used(3-chloro-2-hydroxypropyl)trimethylammonium chloride solution to chemical modify the AL by quaternization.AML-45 was activated in 8g/L NaOH,12g/L urea and-10℃,then in alkaline medium activated AML-45 and polyethylene glycol diglycidyl ether were co-polymerized to prepare lignin-based pH-responsive hydrogel.The structures of AML-45 and ligninbased hydrogel were characterized by FTIR spectroscopy,DLS measurement.Scanning Electron Microscope was used to discover hydrogel’s morphological characteristics.The swelling behavior of the hydrogel at different pH PBS-buffered solution was tracked.These results showed that the hydrogel was highly pH-responsive to a range of pH 2—7.4,with the swelling rate reaching minimum of 260%(pH=4)and maximum of 330%(pH=7.4).In addition,the swelling rate of hydrogel related to the lignin concentration,amount of cross-linker polyethylene glycol diglycidyl ether and 5-fluorouracil was used as model drug to explore its drug release behavior in buffer media in the acidic range(pH=2—7.4).The cumulative drug release from the loaded hydrogel in buffer solution(pH=7.4)was up to 78%within 30h which was higher than the cumulative drug release of 62%(pH=4)and 69%in(pH=2)in acidic buffer environment.The hydrogel had significantly drug retarded effect.

关 键 词：木质素 水凝胶 PH响应性 聚合物 药物 生物质 凝胶 

分 类 号：TQ427.26[化学工程]