pH响应性PAA/毒死蜱/氨基化介孔硅缓释体系的制备与性能

doi:10.11949/j.issn.0438-1157.20160417

化工学报 ›› 2016, Vol. 67 ›› Issue (10): 4500-4507.DOI: 10.11949/j.issn.0438-1157.20160417

• 材料化学工程与纳米技术 • 上一篇下一篇

pH响应性PAA/毒死蜱/氨基化介孔硅缓释体系的制备与性能

林粤顺, 周红军, 周新华, 龚圣, 徐华, 陈铧耀

仲恺农业工程学院化学化工学院, 广东广州 510225

收稿日期:2016-04-05 修回日期:2016-07-24 出版日期:2016-10-05 发布日期:2016-10-05
通讯作者: 周新华
基金资助:
国家自然科学基金项目（21576303）；广东省自然科学基金项目（2016A030313375）；广东省科技计划项目（2014A020208126）；广州市科技计划项目（201510010150）。

Preparation and properties of pH-responsive control release system of PAA/chlorpyrifos/amino functionalized mesoporous silica

LIN Yueshun, ZHOU Hongjun, ZHOU Xinhua, GONG Sheng, XU Hua, CHEN Huayao

College of Chemistry and Chemical Engineering, Zhongkai University of Agriculture and Engineering, Guangzhou 510225, Guangdong, China

Received:2016-04-05 Revised:2016-07-24 Online:2016-10-05 Published:2016-10-05
Supported by:
supported by the National Natural Science Foundation of China (21576303) and the Natural Science Foundation of Guangdong Province (2016A030313375).

摘要/Abstract

摘要：

以共缩聚法合成氨基化介孔硅，采用浸渍法制备毒死蜱/氨基化介孔硅，并以带负电荷的聚丙烯酸（PAA）为功能分子，通过静电吸附作用制备了具有pH响应的PAA/毒死蜱/氨基化介孔硅缓释体系。利用XRD、N₂吸附-脱附、TEM、SEM、TG、Zeta电位和FTIR对PAA/毒死蜱/氨基化介孔硅的结构进行了表征，并探究了其在不同pH和温度下的释药行为。结果表明，PAA通过静电作用包覆于毒死蜱/氨基化介孔硅的表面。缓释体系的药物释放主要受到PAA的阻碍作用，PAA修饰载药氨基化介孔硅显示出明显的pH响应性，当pH≤7时，其药物释放速率随pH减小而增大，而在偏碱性条件下的释药速率稍大于中性环境。同时，载药体系的释药速率还受到温度的影响。其释药行为可用Korsmeryer-Pappas动力学模型来描述。

关键词: 氨基化介孔硅, 聚丙烯酸, pH响应, 毒死蜱, 缓释

Abstract:

A pH-responsive control release system of PAA/chlorpyrifos/mesoporous silica was prepared by using negative charged polyacrylic acid (PAA) to encapsulate amino functionalized mesoporous silica (NH₂-MCM-41) with chlorpyrifos loaded in the pores. The PAA/chlorpyrifos/NH₂-MCM-41 system were systematically characterized using X-ray diffraction (XRD), N₂ adsorption-desorption, transmission electron microscopy (TEM), scanning electron microscopy (SEM), thermogravimetric analysis (TGA), Zeta potential and Fourier transform infrared spectroscopy (FTIR). The release behavior of chlorpyrifos was studied at various pH and temperature conditions. The experimental results showed that PAA was coated on the surface of chlorpyrifos/amino functionalized mesoporous silica as a result of electrostatic interaction. The chlorpyrifos release from the PAA/chlorpyrifos/NH₂-MCM-41 system was inhibited mainly by PAA blockage with significant pH sensitivity, which increased with pH decrease at pH ≤ 7 and was slightly higher in weak base condition than that in neutral condition. The release also exhibited some temperature dependence and generally followed the Korsmeyer-Peppas kinetic model.

Key words: amino functionalized mesoporous silica, PAA, pH-responsive, chlorpyrifos, control release

中图分类号:

TQ450.6

林粤顺, 周红军, 周新华, 龚圣, 徐华, 陈铧耀. pH响应性PAA/毒死蜱/氨基化介孔硅缓释体系的制备与性能[J]. 化工学报, 2016, 67(10): 4500-4507.

LIN Yueshun, ZHOU Hongjun, ZHOU Xinhua, GONG Sheng, XU Hua, CHEN Huayao. Preparation and properties of pH-responsive control release system of PAA/chlorpyrifos/amino functionalized mesoporous silica[J]. CIESC Journal, 2016, 67(10): 4500-4507.

参考文献 27

[1]	ZHAO D Y, HUO Q S, FENG J L, et al. Correction to "Nonionic triblock and star diblock copolymer and oligomeric surfactant syntheses of highly ordered, hydrothermally stable, mesoporous silica structures"[J]. Journal of the American Chemical Society, 2014, 136(29):10546.
[2]	WANG Y, HAN N, ZHAO Q F, et al. Redox-responsive mesoporous silica as carriers for controlled drug delivery:a comparative study based on silica and PEG gatekeepers[J]. European Journal of Pharmaceutical Sciences, 2015, 72(2):12-20.
[3]	PAPAT A, HARTONO S B, STAHR F, et al. Mesoporous silica nanoparticles for bioadsorption, enzyme immobilisation and delivery carriers[J]. Nanoscale, 2011, 3(7):2801-2718.
[4]	TROJER M A, NORDSTIERNA L, NORDIN M, et al. Encapsulation of actives for sustained release[J]. Physical Chemistry Chemical Physics, 2013, 15:17727-17741.
[5]	VALLET-REGI M, RAMILA A, DEL R R P, et al. A new property of MCM-41:drug delivery system[J]. Chemistry of Materials, 2001, 13(2):308-311.
[6]	TIANABC Y, KONGD Y, LIG X, et al. Light and pH-activated intracellular drug release from polymeric mesoporous silica nanoparticles[J]. Colloids and Surfaces B Biointerfaces, 2015, 134:147-155.
[7]	GUO W, YANG C, CUI L, et al. An enzyme-responsive controlled release system of mesoporous silica coated with Konjac oligosaccharide[J]. Langmuir, 2014, 30(1):243-249.
[8]	ALBERTI S, SOLER I G J A A, AZZARONI O. Gated supramolecular chemistry in hybrid mesoporous silica nanoarchitectures:controlled delivery and molecular transport in response to chemical, physical and biological stimuli[J]. Chemical Communications, 2015, 51(28):6050-6075.
[9]	CHEN F, JIANG, X P, KUAN T R, et al. Polyelectrolyte/mesoporous silica hybrid materials for the high performance multiple-detection of pH value and temperature[J]. Polymer Chemistry, 2015, 6(18):3529-3536.
[10]	YUAN L, TANG Q, YANG D, et al. Preparation of pH-responsive mesoporous silica nanoparticles and their application in controlled drug delivery[J]. The Journal of Physical Chemistry C, 2011, 115(20):9926-9932.
[11]	BILALIS P, TZIBELEKA L, VARLASA S, et al. pH-Sensitive nanogates based on poly(L-histidine) for controlled drug release from mesoporous silica nanoparticles[J]. Polymer Chemistry, 2016, 7(7):1475-1485.
[12]	POURJAVADI A, TEHRANI Z M, BENNETT C. PEG-co-polyvinyl pyridine coated magnetic mesoporous silica nanoparticles for pH-responsive controlled release of doxorubicin[J]. International Journal of Polymeric Materials, 2015, 64(11):570-577.
[13]	郭月月, 白诗扬, 孙继红. pH敏感型双模型介孔SiO2的制备及其对布洛芬的缓控释性能[J]. 石油学报(石油加工), 2014, 30(1):181-186. GUO Y Y, BAI S Y, SUN J H. Preparation of pH-responsive bimodal mesoporous silicas and their performances in controlled ibuprofen delivery[J]. Acta Petrolei Sinica(Petroleum Processing Section), 2014, 30(1):181-186.
[14]	WIBOWO D, ZHA C X, PETERS B C, et al. Sustained release of fipronil insecticide in vitro and in vivo from biocompatible silica nanocapsules[J]. Journal of Agricultural and Food Chemistry, 2014, 62(52):12504-12511.
[15]	PRADO A G S, MOURA A O, NUNES A R. Nanosized silica modified with carboxylic acid as support for controlled release of herbicides[J]. Journal of Agricultural and Food Chemistry, 2011, 59(16):8847-8852.
[16]	WAN M M, YANG J Y, QIU Y,et al. Sustained release of heparin on enlarged-pore and functionalized MCM-41[J]. Applied Materials & Interfaces, 2012, 4(8):4113-4122.
[17]	彭仁忠. 控制释放技术在植物病虫害防治中的应用[J]. 北京农业, 2014, (15):112. PENG R Z. Application of controlled release technology in the control of plant diseases and insect pests[J]. Beijing Agriculture, 2014, (15):112.
[18]	GAURAV J, ANOOP N, ABDUR R, et al. Fluoride ion sensing in aqueous medium by employing nitrobenzoxadiazole-postgrafted mesoporous silica nanoparticles (MCM-41)[J]. Physical Chemistry Chemical Physics, 2015, 17(5):3525-3533.
[19]	GU J, FAN W, SHIMOJIMA A, et al. Organic-inorganic mesoporous nanocarriers integrated with biogenic ligands[J]. Small, 2007, 3(10):1740-1744.
[20]	ROSTAMIZADEH S, NOJAVAN M. An environmentally benign multicomponent synthesis of some novel 2-methylthio pyrimidine derivatives using MCM-41-NH2 as nanoreactor and nanocatalyst[J]. Journal of Heterocyclic Chemistry, 2014, 51(2):418-422.
[21]	林粤顺, 周新华, 周红军, 等. 毒死蜱/羽毛蛋白/海藻酸钠复合微球的制备及其缓释性能)[J]. 农药, 2014, 30(12):892-896, 911. LIN Y S, ZHOU X H, ZHOU H J, et al. Preparation and slow-release performance of chlorpyrifos/feather keratin/sodium alginate microspheres[J]. Agrochemicals, 2014, 30(12):892-896, 911.
[22]	ZENG W, QIAN X, YIN J, et al. The drug delivery system of MCM-41 materials via co-condensation synthesis[J]. Materials Chemistry and Physics, 2006, 97(2/3):437-441.
[23]	HARTONO S B, QIAO S Z, JACK K, et al. Improving adsorbent properties of cage-like ordered amine functionalized mesoporous silica with very large pores for bioadsorption[J]. Langmuir, 2009, 25(11):6413-6424.
[24]	岳林海, 金达莱. 两亲PS-b-PAA共聚物水溶液中球形碳酸钙复合物的合成及其热分解性质[J]. 科学通报, 2004, 49(1):61-64. YUE L H, JIN D L. Synthesis and thermal decomposition properties of spherical calcium carbonate complex in aqueous solution of amphiphilic PS-b-PAA[J]. Chinese Science Bulletin, 2004, 49(1):61-64.
[25]	周细应, 李卫红, 何亮. 纳米颗粒的分散稳定性及其评估方法[J]. 材料保护, 2006, 39(6):51-54. ZHOU X Y, LI W H, HE L. Dispersion stability of nanoparticles and its evaluation methods[J]. Materials Protection, 2006, 39(6):51-54.
[26]	DASH S, MURTHY P N, NATH L, et al. Kinetic modeling on drug release from controlled drug delivery systems[J]. Acta Poloniae Pharmaceutica-Drug Research, 2010, 67(3):217-223.
[27]	HONG C Y, LI X, PAN C Y. Fabrication of smart nanocontainers with a mesoporous core and a pH-responsive shell for controlled uptake and release[J]. Journal of Materials Chemistry, 2009, 19(29):5155-5160.

pH响应性PAA/毒死蜱/氨基化介孔硅缓释体系的制备与性能

Preparation and properties of pH-responsive control release system of PAA/chlorpyrifos/amino functionalized mesoporous silica

PDF (PC)

可视化

被引次数

摘要/Abstract

引用本文

使用本文

参考文献 27

相关文章 15

编辑推荐

Metrics

本文评价

[1]	王德宏, 孙琳, 罗雄麟. 海水淡化系统多效蒸发传热温差全周期渐变优化分析[J]. 化工学报, 2022, 73(12): 5469-5482.
[2]	邱松发, 许斌华, 林冠权, 周新华, 陈铧耀, 周红军. 2,4-D/CMC接枝物纳米粒子的制备与缓释性能研究[J]. 化工学报, 2019, 70(5): 2007-2015.
[3]	陈政, 王莉, 周健. 双响应性嵌段聚合物的纳米孔开关效应的计算机模拟[J]. 化工学报, 2019, 70(1): 271-279.
[4]	周红军, 林粤顺, 李舒静, 徐华, 陈铧耀, 周新华. 席夫碱锌改性介孔硅对毒死蜱的吸附与缓释[J]. 化工学报, 2018, 69(5): 2272-2281.
[5]	杨东杰, 施一鸣, 单国荣. 丙烯酸酯用量对溶胀-嵌段型水性聚氨酯性能的影响[J]. 化工学报, 2018, 69(11): 4856-4861.
[6]	李婷婷, 赵乐乐, 郑子良, 王振军, 张瑞平. 右旋布洛芬/尿素改性蒙脱土复合物的制备及体外释药性能[J]. 化工学报, 2017, 68(9): 3631-3637.
[7]	周枫, 李智宇, 李根, 江涛, 者为, 黄艳, 卢真保, 李忠. 茴香醚在葡萄糖基多孔碳材料上缓释机理[J]. 化工学报, 2017, 68(12): 4625-4632.
[8]	杜朋亚, 边锋, 姚蒙蒙, 常达, 唐二军. 高阻尼性涂层用环氧-丙烯酸酯复合乳液的合成[J]. 化工学报, 2016, 67(10): 4508-4513.
[9]	周守勇, 薛爱莲, 张艳, 王启伟, 李梅生, 褚效中, 赵宜江, 邢卫红. 聚丙烯酸改性凹土对Pb²⁺、Ni²⁺和Cr³⁺的选择性吸附[J]. 化工学报, 2015, 66(2): 618-625.
[10]	吴洁, 丁师杰, 陈静, 蒋金龙, 王军军. 酸化凹凸棒石/海藻酸复合材料的制备及其缓释性能[J]. 化工学报, 2014, 65(11): 4627-4632.
[11]	吴文果1，2，刘伟1，王士斌1，2，刘源岗1，2，陈爱政1，2. 海藻酸钙/聚精氨酸微胶囊的载药和缓释性能[J]. 化工进展, 2014, 33(05): 1271-1275.
[12]	李利军，崔越，李青松，刘焘，李彦青. 赤砂糖回溶糖浆的半碳法澄清脱色工艺[J]. 化工进展, 2013, 32(08): 1755-1758.
[13]	刘源岗1，2，郑琪瑶1，王士斌1，2. 盐酸米托蒽醌多囊脂质体的制备工艺优化及性能[J]. 化工进展, 2013, 32(06): 1395-1400.
[14]	阚文涛1，李欣2，罗顺忠1，胡睿1. 印迹水凝胶作为氟尿嘧啶载体的药物缓释性能[J]. 化工进展, 2013, 32(03): 627-633.
[15]	徐婷婷，李治方，吴洁，陈静. 缓释铜的凹土/海藻酸钠复合微球的制备及性能测试[J]. 化工进展, 2013, 32(02): 410-413.