化学学报 ›› 2014, Vol. 72 ›› Issue (8): 963-969.DOI: 10.6023/A14030146 上一篇    

研究论文

喜树碱/氧化石墨烯/类水滑石纳米杂化物的制备及表征

兀晓文, 杜娜, 李海平, 张人杰, 侯万国   

  1. 山东大学胶体与界面化学教育部重点实验室 济南 250100
  • 收稿日期:2014-03-04 出版日期:2014-08-14 发布日期:2014-06-03
  • 通讯作者: 侯万国 E-mail:wghou@sdu.edu.cn
  • 基金资助:
    项目受国家自然科学基金(Nos. 21173135,21273135)和高等学校博士学科点专项科研基金(No. 20110131130008)资助.

Synthesis and Characterization of Camptothecin/Graphene Oxide/Hydrotalcite-like Compounds Nanohybrids

Wu Xiaowen, Du Na, Li Haiping, Zhang Renjie, Hou Wanguo   

  1. Key Laboratory of Colloid and Interface Chemistry Ministry of Education, Shandong University, Jinan 250100, China
  • Received:2014-03-04 Online:2014-08-14 Published:2014-06-03
  • Supported by:
    Project supported by the National Natural Science Foundation of China (Nos. 21173135, 21273135) and the Specialized Research Fund for the Doctoral Program of Higher Education of China (No. 20110131130008)

采用共组装法成功制备了电中性疏水抗癌药物喜树碱(CPT)/氧化石墨烯(GO)/Mg-Al类水滑石(HTlc)纳米杂化物. 先将CPT负载于荷负电的GO纳米片表面上制备成CPT/GO复合物,再与荷正电的HTlc纳米片(HNS)共组装,形成CPT/GO/HTlc纳米杂化物,其中GO纳米片和HNS相间叠加,CPT负载于层间. 采用X-射线衍射、透射电子显微镜、原子力显微镜、扫描电子显微镜-能量色谱仪、傅里叶变换红外光谱、紫外-可见分光光度计和热重/差示扫描量热分析等技术对纳米杂化物进行了表征. 37 ℃下分别在pH 7.4和4.0的磷酸缓冲液中,考察了CPT/GO/HTlc纳米杂化物的药物释放行为. 结果表明,CPT/GO/HTlc纳米杂化物的药物释放过程符合准二级动力学方程,且具pH响应性,在酸性(pH 4.0)介质中的释放速率和释放率明显高于中性(pH 7.4)介质. 共组装法是构筑药物/ GO/HTlc纳米杂化物的简便方法,该纳米杂化物在药物输送领域具有良好的应用前景.

关键词: 类水滑石, 氧化石墨烯, 喜树碱, 药物释放, 共组装

A nanohybrid of the charge-neutral and poorly water-soluble anticancer drug camptothecin (CPT)/graphene oxide (GO)/Mg-Al hydrotalcite-like compounds (HTlc) was synthesized using a coassembly route. For the coassembly route, CPT molecules were initially loaded on the surface of GO nanosheets; the resulting negatively charged CPT-loaded GO nanosheets and the positively charged HTlc nanosheets were then coassembled together into the layered CPT/GO/HTlc nanohybrid, in which the GO nanosheets and the HTlc nanosheets were alternatively stacked and the CPT molecules were located in its interlayer gallery. The so-obtained nanohybrid was characterized using X-ray diffraction, transmission electron microscope, atomic force microscope, scanning electron microscope-energy dispersive spectrometer, Fourier transform infrared spectrometer, ultraviolet-visible spectrophotometry and thermogravimetric analysis/differential scanning calorimetry technique. The mass ratio of GO to HTlc nanosheets in the nanohybrid was 0.63. The loading amount of CPT on the GO nanosheets was 61.0 mg/g, and that in the nanohybrid was 13.4 mg/g. The d-spacing of the CPT/GO composite and the nanohybrid were 0.84 and 1.35 nm, respectively. The in vitro release of CPT from the nanohybrid was examined in pH 7.4 and 4.0 phosphate buffer solutions at 37 ℃. The results showed that the drug release process could be described with pseudo-second order kinetic model, and exhibited strong pH dependence, namely, the release rate and the percentage release in pH 4.0 buffer were evidently higher than those in pH 7.4 buffer. The pH dependence of CPT release is due to a possible difference in the release mechanism. The CPT release in pH 7.4 buffer was a diffusion-controlled process and the intraparticle diffusion was the rate-limiting step; in pH 4.0 buffer, the dissolution of HTlc layers and the weakening of π-π interaction between CPT and GO also played an important role for CPT release. The maximum percentage releases of CPT from the nanohybrid in pH 7.4 and 4.0 buffers were about 26.8% and 31.1%, respectively, higher than that from CPT/GO composites. The coassembly method is a simple route for building drug/GO/HTlc nanohybrids, and the nanohybrids have potential applications in drug delivery.

Key words: hydrotalcite-like compounds, graphene oxide, camptothecin, drug release, coassembly