化工进展 ›› 2023, Vol. 42 ›› Issue (6): 3138-3146.DOI: 10.16085/j.issn.1000-6613.2023-0074

• 材料科学与技术 • 上一篇    下一篇

pH响应性木质素水凝胶的制备及药物控释

于丁一(), 李圆圆(), 王晨钰, 纪永升   

  1. 河南中医药大学药学院,河南 郑州 450046
  • 收稿日期:2023-01-15 修回日期:2023-03-21 出版日期:2023-06-25 发布日期:2023-06-29
  • 通讯作者: 李圆圆
  • 作者简介:于丁一(1997—),男,硕士研究生,研究方向为生物质基高分子材料。E-mail:2571683628@qq.com
  • 基金资助:
    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)

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

YU Dingyi(), LI Yuanyuan(), WANG Chenyu, JI Yongsheng   

  1. College of Pharmacy, Henan University of Chinese Medicine, Zhengzhou 450046, Henan, China
  • Received:2023-01-15 Revised:2023-03-21 Online:2023-06-25 Published:2023-06-29
  • Contact: LI Yuanyuan

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。

关键词: 木质素, 水凝胶, pH响应性, 聚合物, 药物, 生物质, 凝胶

Abstract:

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 lignin-based 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.

Key words: lignin, hydrogel, pH responsiveness, polymers, pharmaceuticals, biomass, gels

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