pH值响应性毒死蜱/铜席夫碱配合物改性SBA-15的制备及缓释性能
Preparation and Properties of pH Value-Responsive Sustained Release System of Chlorpyrifos/Copper(Ⅱ)) Schiff Base SBA-15
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林粤顺 仲恺农业工程学院化学化工学院, 广州市农用化学品高效利用重点实验室, 广州 510225  
周红军 仲恺农业工程学院化学化工学院, 广州市农用化学品高效利用重点实验室, 广州 510225  
周新华 仲恺农业工程学院化学化工学院, 广州市农用化学品高效利用重点实验室, 广州 510225 cexinhuazhou@163.com 
龚圣 仲恺农业工程学院化学化工学院, 广州市农用化学品高效利用重点实验室, 广州 510225  
徐华 仲恺农业工程学院化学化工学院, 广州市农用化学品高效利用重点实验室, 广州 510225  
陈铧耀 仲恺农业工程学院化学化工学院, 广州市农用化学品高效利用重点实验室, 广州 510225  
摘要: 以3-氨丙基三乙氧基硅烷(APTES)、水杨醛和铜离子为改性剂,通过后嫁接法制得铜席夫碱配合物改性SBA-15(Cu-SBA-15),并以毒死蜱为模型药物,制备了毒死蜱/铜席夫碱配合物改性SBA-15缓释体系。利用TEM、SEM、XRD、N2吸附-脱附、TG、FTIR和XPS对SBA-15、氨基改性SBA-15(NH2-SBA-15)、水杨醛希夫碱改性SBA-15(SA-SBA-15)的形貌、结构和Cu-SBA-15的配位情况进行了表征,考察了SBA-15在改性前后对毒死蜱的吸附量和缓释性能,并着重探究了毒死蜱/铜席夫碱配合物改性SBA-15载药体系在不同pH值下的释药行为。结果表明,APTES和水杨醛能够通过后嫁接法修饰于SBA-15,修饰后仍保持十分有序的孔道结构。SBA-15通过改性后,其对毒死蜱的吸附量由100 mg·g-1增加至195 mg·g-1,且其对药物的缓释性能也得到改善。毒死蜱/铜席夫碱配合物改性SBA-15缓释体系显示出明显的pH值响应性,pH=3时的释药速率大于pH=11时,而在中性条件下的缓释效果相对最好。载药体系的释药行为可用Riger-Peppas动力学模型来描述,其药物释放由Fick扩散控制。
关键词: SBA-15  铜席夫碱  pH值响应  毒死蜱  缓释
基金项目: 国家自然科学基金(No.21576303,21606262)、广东省自然科学基金(No.2016A030313375)、广东省科技计划(No.2015A020209197)和广州市科技计划(No.201510010150)资助项目。
Abstract: Copper Schiff base modified SBA-15(Cu-SBA-15) was prepared by post-grafting, using 3-aminopropyl triethoxysilane (APTES), salicylaldehyde and copper ions as modifying agent. The chlorpyrifos/Cu-SBA-15 (CH-Cu-SBA-15) system were prepared by impregnation method, employing chlorpyrifos as a model drug. The morphologies and structures of SBA-15, amino functionalized SBA-15(NH2-SBA-15), salicylaldehyde functionalized SBA-15(SA-SBA-15), and Cu-SBA-15 were systematically characterized by transmission electron microscopy(TEM), scanning electron microscopy(SEM), X-ray diffraction assay(XRD), N2 adsorption-desorption, TGA analysis, Fourier transform infrared spectroscopy(FTIR) and X-ray photoelectron spectroscopy(XPS). Meanwhile, the adsorption capacity(AC) of as-synthesized system for chlorpyrifos and sustained release performance of SBA-15 before and after modification were investigated. Besides, the sustained release behavior of CH-Cu-SBA-15 under different pH values were also discussed. The results showed that SBA-15 could be modified by APTES and salicylaldehyde, and the order structure of it was still maintained by post-grafting method. After modification of SBA-15, the AC of chlorpyrifos increased from 100 to 195 mg·g-1 with a better sustained release performance. In addition, the CH-Cu-SBA-15 system showed significant sensitivity in response to the pH value. The chlorpyrifos release rate under pH=3 was greater than pH=11 and the sustained release performance of them was relatively better than under the neutral condition. Meanwhile, their releasing curves could be described by Riger-Peppas equation indicating that the drug release was controlled by Fick diffusion.
Keywords: SBA-15  copper(Ⅱ) Schiff base  pH value responsiveness  chlorpyrifos  sustained release
投稿时间:2016-11-10 修订日期:2016-12-25
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林粤顺,周红军,周新华,龚圣,徐华,陈铧耀.pH值响应性毒死蜱/铜席夫碱配合物改性SBA-15的制备及缓释性能[J].无机化学学报,2017,33(3):446-454.
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