半纤维素基阿维菌素载药微囊的制备及性能

doi:10.16085/j.issn.1000-6613.2019-1552

摘要/Abstract

摘要：

目前阿维菌素以高效性、无污染和低抗药性等特点而得到广泛应用，但是其稳定性较差，易降解导致使用量较大从而造成浪费。为解决上述问题，本文以半纤维素为基体，利用原位聚合法制备阿维菌素载药微囊（HDCM），通过制备条件、热降解性、储存稳定性和释放动力学研究，确定了HDCM的载药量、热稳定性及释放性能。结果表明，在芯壁比为1∶34（质量比），温度为65℃，pH为3.5的制备条件下，HDCM的载药量可达66.5%，粒径较小且分散均匀。HDCM的热降解性能和恒温热稳定性能较阿维菌素原药有所提高，最高热分解温度从261℃增加到272℃，阿维菌素原药10h后降解率达到12.1%，而载药量为66.5%的HDCM降解率仅为5.2%。HDCM的释放机理满足Fick扩散，阿维菌素原药在水中的累积释放率在12h之内达到83.8%，而HDCM的累积释放率在24h之后才有所增大，12h内其释放率仅为33.7%，表明HDCM具有极好的缓释性能。

关键词: 半纤维素, 阿维菌素, 聚合, 载体, 降解

Abstract:

Abamectin has been widely used due to its high efficiency, pollution-free, and less drug resistance, but its poor stability and easy degradation lead to a large amount of utilization and waste. To solve the problems, abamectin-loaded microcapsule (HDCM) based on hemicellulose was prepared by in-situ polymerization. By studying preparation conditions, thermal degradation, storage stability and release kinetics, drug loading, thermal stability and release performances of HDCM were determined. The results showed that the drug loading of HDCM could reach 66.5%, and it had small particle size and uniform dispersion under the preparation conditions of the core-wall mass ratio of 1∶34, temperature of 65℃ and pH of 3.5. The thermal degradation performance and constant temperature thermal stability of HDCM were improved compared to avermectin agent. The maximum temperature of thermal decomposition was increased from 261℃ to 272℃. After 10h, the degradation rate of avermectin agent reached 12.1%, and the degradation rate of HDCM with the drug loading of 66.5% was only 5.2%. The release mechanism on HDCM satisfies Fick diffusion. The cumulative release rate of avermectin agent in water reached 83.8% within 12h, while the cumulative release rate of HDCM gradually increased after 24h. Within 12h the release rate of HDCM was only 33.7%, indicating that HDCM had excellent sustained release performance.

Key words: hemicellulose, abamectin, polymerization, support, degradation

中图分类号:

TQ319

张林雅, 薛伟, 顾丽敏. 半纤维素基阿维菌素载药微囊的制备及性能[J]. 化工进展, 2020, 39(8): 3246-3255.

Linya ZHANG, Wei XUE, Limin GU. Study on preparation and properties of hemicellulose abamectin-loaded microcapsule[J]. Chemical Industry and Engineering Progress, 2020, 39(8): 3246-3255.

参考文献

1	高海龙, 刘娜, 傅英娟, 等. 半纤维素功能材料的研究进展[J]. 造纸科学与技术, 2017, 36(6): 24-28.
1	GAO Hailong, LIU Na, FU Yingjuan, et al. Research progress of hemicellulose functional materials[J]. Paper Science and Technology, 2017, 36(6): 24-28.
2	刘冉, 李育峰, 李海明, 等. 半纤维素在食品包装材料中的应用及研究进展[J]. 中华纸业, 2018, 39(8): 6-11.
2	LIU Ran, LI Yufeng, LI Haiming, et al. Application and research progress of hemicellulose in food packaging materials[J]. China Pulp and Paper Industry, 2018, 39(8): 6-11.
3	程合丽, 冯清华, 陈洪雷, 等. 半纤维素基水凝胶制备方法研究进展[J]. 造纸科学与技术, 2015, 34(6): 40-45.
3	CHENG Heli, FENG Qinghua, CHEN Honglei, et al. Research progress in preparation methods of hemicellulose-based hydrogels[J]. Paper Science and Technology, 2015, 34(6): 40-45.
4	徐扣峰, 孙健, 吴静. 半纤维素水凝胶的制备及功能性研究[J]. 广东化工, 2018, 45(8): 50, 60-61.
4	XU Koufeng, SUN Jian, WU Jing. Preparation and functional study of hemicellulose hydrogels[J]. Guangdong Chemical Industry, 2018, 45(8): 50, 60-61.
5	周帅, 苗庆显, 黄六莲, 等. 木质纤维生物质半纤维素基功能材料研究进展[J]. 林产化学与工业, 2017, 37(6): 1-10.
5	ZHOU Shuai, MIAO Qingxian, HUANG Liulian, et al. Research progress of lignocellulosic biomass hemicellulose-based functional materials[J]. Chemistry and Industry of Forest Products, 2017, 37 (6): 1-10.
6	张林雅, 于捍江. 季铵半纤维素分散剂的合成及应用[J]. 精细化工, 2014, 31(11): 1306-1309.
6	ZHANG Linya, YU Hanjiang. Synthesis and application of quaternary ammonium hemicellulose dispersant[J]. Fine Chemicals, 2014, 31(11): 1306-1309.
7	张林雅. 羧甲基半纤维素钠分散炭黑色浆的制备研究[J]. 印染助剂, 2017, 34(5): 12-15.
7	ZHANG Linya. Study on preparation of carbon black pulp dispersed by sodium carboxymethyl hemicellulose[J]. Textile Auxiliaries, 2017, 34(5): 12-15.
8	ZHANG Linya, XUE Wei, GU Limin. Modification of hyperbranched hemicellulose polymer and its application in adsorbing acid dyes[J]. Cellulose, 2019, 26(9): 5583-5601.
9	郑瑾, 王杨柳, 王帅, 等. 原位微悬浮聚合法制备姜黄色素微胶囊[J]. 上海纺织科技, 2019, 47(1): 24-27.
9	ZHENG Jin, WANG Yangliu, WANG Shuai, et al. Preparation of turmeric pigment microcapsules by in-situ microsuspension polymerization[J]. Shanghai Textile Science and Technology, 2019, 47(1): 24-27.
10	李薇, 何源. 微胶囊技术在智能纺织品上的应用[J]. 上海纺织科技, 2019, 47(12): 1-21.
10	LI Wei, HE Yuan. Application of microcapsule technology in smart textiles[J]. Shanghai Textile Science and Technology, 2019, 47(12): 1-21.
11	程璐璐, 杨建森, 曹向阳, 等. 原位聚合法制备微胶囊相变材料及热工性能研究[J]. 新型建筑材料, 2019, 46(7): 89-93.
11	CHENG Lulu, YANG Jiansen, CAO Xiangyang, et al. Preparation of microencapsulated phase change materials by in-situ polymerization and study on thermal properties[J]. New Building Materials, 2019, 46(7): 89-93.
12	张倩, 刘姝岩, 王中伟, 等. 多糖及其衍生物在食品微胶囊壁材中的应用[J]. 中国食品添加剂, 2019, 30(11): 132-137.
12	ZHANG Qian, LIU Shuyan, WANG Zhongwei, et al. Application of polysaccharides and their derivatives in food microcapsule wall materials[J]. China Food Additives, 2019, 30(11): 132-137.
13	杨晓军, 赵李阳, 李青阳, 等. 乳液稳定性对溶剂挥发法制备微胶囊的影响[J]. 北京工业大学学报, 2020, 46(2): 199-207.
13	YANG Xiaojun, ZHAO Liyang, LI Qingyang, et al. Effect of emulsion stability on microcapsules prepared by solvent volatilization[J]. Journal of Beijing University of Technology, 2020, 46(2): 199-207.
14	钟玲, 张世玲, 任华, 等. 高含量阿维菌素微囊悬浮剂的制备[J]. 现代农药, 2019, 18(5): 15-17.
14	ZHONG Ling, ZHANG Shiling, REN Hua, et al. Preparation of high-content avermectin microcapsule suspension[J]. Modern Agrochemicals, 2019, 18(5): 15-17.
15	李飞, 韩冲冲, 李保同. 阿维菌素无人机喷施的沉积特征及防效研究[J]. 江西农业大学学报, 2019, 41(5): 914-923.
15	LI Fei, HAN Chongchong, LI Baotong. Study on the deposition characteristics and control effects of avermectin drone spraying[J]. Journal of Jiangxi Agricultural University, 2019, 41(5): 914-923.
16	陈龙, 周红军, 江海科, 等. 叶面亲和型阿维菌素微胶囊的制备及pH响应性释放性能[J]. 化工进展, 2020, 39(1): 348-355.
16	CHEN Long, ZHOU Hongjun, JIANG Haike, et al. Preparation of foliar affinity avermectin microcapsules and its pH-responsive release properties[J]. Chemical Industry and Engineering Progress, 2020,39(1): 348-355.
17	宋云飞, 娄鸿飞, 吕绪良, 等. 原位聚合法制备微胶囊的研究进展[J]. 化工新型材料, 2018, 46(9): 30-40.
17	SONG Yunfei, LOU Hongfei, Xuliang LYU, et al. Research progress of microcapsule preparation by in-situ polymerization[J]. New Chemical Materials, 2018, 46(9): 30-40.
18	杨晓娜, 于建新, 甘志勇, 等. 表面活性剂对原位聚合法合成微胶囊的影响[J]. 粘接, 2015, 36(5): 56-60.
18	YANG Xiaona, YU Jianxin, GAN Zhiyong, et al. Effect of surfactants on microcapsules preparing process via in situ polymerization[J]. Adhesion, 2015, 36(5): 56-60.
19	王镭, 赵静. 脲醛树脂胶粘剂制备毒死蜱微胶囊[J]. 北京化工大学学报(自然科学版), 2009, 36(5): 46-51.
19	WANG Lei, ZHAO Jing. Preparation of chlorpyrifos microcapsules with urea-formaldehyde resin adhesive[J]. Journal of Beijing University of Chemical Technology (Natural Science Edition), 2009, 36(5): 46-51.
20	彭涛. 脲醛树脂微胶囊的制备及其摩擦磨损性能研究[D]. 湘潭: 湖南科技大学, 2015.
20	PENG Tao. Preparation of urea formaldehyde resin microcapsules and study on their friction and wear properties[D]. Xiangtan: Hunan University of Science and Technology, 2015.
21	ANETA Cymbaluk P?oska, PETER Sobolewski, ANITA Chudecka G?az, et al. Double-emulsion copolyester microcapsules for sustained intraperitoneal release of carboplatin[J]. Journal of Functional Biomaterials, 2019, 10(4): 10040055.
22	ELESINI Ur?ka S, Jernej ?VARC, Bo?tjan ?UMIGA, et al. Melamine formaldehyde microcapsules with fragrance core material: preparation, properties, and end use[J]. Journal of Textile Research, 2017, 87(20): 2435-2448.
23	CESARI Adriana, LOUREIRO Mónica V, Mário VALE, et al. Polycaprolactone microcapsules containing citric acid and naringin for plant growth and sustainable agriculture: physico-chemical properties and release behavior[J]. Science of the Total Environment, 2020, 703: 135548.
24	李舣. 阿维菌素—毒死蜱复配农药微胶囊的制备与性能[D]. 长沙: 湖南农业大学, 2013.
24	LI Yi. Preparation and performance of avermectin-chlorpyrifos compound pesticide microcapsules[D]. Changsha: Hunan Agricultural University, 2013.
25	GAUCHER Geneviève, DUFRESNE Marie Hélène, SANT Vinayak P, et al. Block copolymer micelles: preparation, characterization and application in drug delivery[J]. Journal of Controlled Release, 2005, 109(1/2/3): 169-188.
26	曾楚楚, 娄钧翼, 郭明, 等. 防治核桃干腐病的新型纳米生物基农药缓释胶囊制备及缓释性能[J]. 林业科学, 2018, 54(5): 87-100.
26	ZENG Chuchu, LOU Junyi, GUO Ming, et al. Preparation and sustained release properties of novel nano-bio-based pesticide sustained-release capsules for preventing and controlling dried walnut rot[J]. Scientia Silvae Sinicae, 2018, 54(5): 87-100.
27	VOJTECH Kundrat, NICOLE Cernekova, ADRIANA Kovalcik, et al. Drug release kinetics of electrospun PHB meshes[J]. Materials, 2019, 12(12): 121924.
28	YU Shouwu, XIAO Shujuan, ZHAO Zewen, et al. Microencapsulated ammonium polyphosphate by polyurethane with segment of dipentaerythritol and its application in flame retardant polypropylene[J]. Chinese Journal of Chemical Engineering, 2019, 27: 1735-1743.
29	RAN Guowen, LIU Xiaodong, GUO Jia, et al. Improving the flame retardancy and water resistance of polylactic acid by introducing polyborosiloxane microencapsulated ammonium polyphosphate[J]. Composites Part B: Engineering, 2019, 173: 106772.
30	CASTELLANO Angela, COLLEONI Claudio, IACONO Giuseppina, et al. Synthesis and characterization of a phosphorous/nitrogen based sol-gel coating as a novel halogen- and formaldehyde-free flame retardant finishing for cotton fabric[J]. Polymer Degradation and Stability, 2019, 162: 148-159.
31	ZHU Zongmin, WANG Luoxin, DONG Liangping. Influence of a novel P/N-containing oligomer on flame retardancy and thermal degradation of intumescent flame-retardant epoxy resin[J]. Polymer Degradation and Stability, 2019, 162: 129-137.
32	ZHANG Aitang, JUNG Kenward, LI Aihua, et al. Recent advances in stimuli-responsive polymer systems for remotely controlled drug release[J]. Progress in Polymer Science, 2019, 99: 101164.
33	SAGITHA P, RESHMI C R, SUNDARAN S P, et al. In-vitro evaluation on drug release kinetics and antibacterial activity of dextran modified polyurethane fibrous membrane[J]. International Journal of Biological Macromolecules, 2018, 126: 717-730.

[1]	高彦静. 单原子催化技术国际研究态势分析[J]. 化工进展, 2023, 42(9): 4667-4676.
[2]	葛全倩, 徐迈, 梁铣, 王凤武. MOFs材料在光电催化领域应用的研究进展[J]. 化工进展, 2023, 42(9): 4692-4705.
[3]	林晓鹏, 肖友华, 管奕琛, 鲁晓东, 宗文杰, 傅深渊. 离子聚合物-金属复合材料（IPMC）柔性电极的研究进展[J]. 化工进展, 2023, 42(9): 4770-4782.
[4]	朱传强, 茹晋波, 孙亭亭, 谢兴旺, 李长明, 高士秋. 固体高分子脱硝剂选择性非催化还原NO _x 特性[J]. 化工进展, 2023, 42(9): 4939-4946.
[5]	李伯耿, 罗英武, 刘平伟. 聚合物产品工程研究内容与方法的思考[J]. 化工进展, 2023, 42(8): 3905-3909.
[6]	王报英, 王皝莹, 闫军营, 汪耀明, 徐铜文. 聚合物包覆膜在金属分离回收中的研究进展[J]. 化工进展, 2023, 42(8): 3990-4004.
[7]	杨静, 李博, 李文军, 刘晓娜, 汤刘元, 刘月, 钱天伟. 焦化污染场地中萘降解菌的分离及降解特性[J]. 化工进展, 2023, 42(8): 4351-4361.
[8]	储甜甜, 刘润竹, 杜高华, 马嘉浩, 张孝阿, 王成忠, 张军营. 有机胍催化脱氢型RTV硅橡胶的制备和可降解性能[J]. 化工进展, 2023, 42(7): 3664-3673.
[9]	于静文, 宋璐娜, 刘砚超, 吕瑞东, 武蒙蒙, 冯宇, 李忠, 米杰. 一种吲哚基超交联聚合物In-HCP对水中碘的吸附作用[J]. 化工进展, 2023, 42(7): 3674-3683.
[10]	徐伟, 李凯军, 宋林烨, 张兴惠, 姚舜华. 光催化及其协同电化学降解VOCs的研究进展[J]. 化工进展, 2023, 42(7): 3520-3531.
[11]	于志庆, 黄文斌, 王晓晗, 邓开鑫, 魏强, 周亚松, 姜鹏. B掺杂Al₂O₃@C负载CoMo型加氢脱硫催化剂性能[J]. 化工进展, 2023, 42(7): 3550-3560.
[12]	龚鹏程, 严群, 陈锦富, 温俊宇, 苏晓洁. 铁酸钴复合碳纳米管活化过硫酸盐降解铬黑T的性能及机理[J]. 化工进展, 2023, 42(7): 3572-3581.
[13]	余希希, 张金帅, 雷文, 刘承果. 基于动态共价键自修复的光固化高分子材料研究进展[J]. 化工进展, 2023, 42(7): 3589-3599.
[14]	于丁一, 李圆圆, 王晨钰, 纪永升. pH响应性木质素水凝胶的制备及药物控释[J]. 化工进展, 2023, 42(6): 3138-3146.
[15]	杨发容, 顾丽莉, 刘洋, 李伟雪, 蔡洁云, 王惠平. 计算机模拟辅助特丁津分子印迹聚合物的制备及应用[J]. 化工进展, 2023, 42(6): 3157-3166.