叶面亲和型阿维菌素微胶囊的制备及pH响应性释放性能

doi:10.16085/j.issn.1000-6613.2019-0661

摘要/Abstract

摘要：

为减少农药流失，设计了一种叶面亲和型缓释微胶囊。以甲基丙烯酸甲酯（MMA）接枝改性羧甲基纤维素（CMC）得到羧甲基纤维素-聚甲基丙烯酸甲酯（CMC-g-PMMA），然后利用自组装负载阿维菌素（AVM）形成载药微胶囊（CMC-g-PMMA@AVM），通过多巴胺（DA）包覆提高CMC-g-PMMA@AVM的叶面亲和性。采用扫描电镜、红外光谱、热重分析等对其结构和形貌进行表征，研究了微胶囊的载药性能、叶面亲和性及响应释放性能。结果显示，DA/CMC-g-PMMA@AVM为平均粒径126nm的球形粒子，多巴胺的包覆可有效提高微胶囊的载药性能，包封率可达88.56%；增强AVM的叶面亲和性，使其叶面滞留量相对于阿维菌素水乳液提升30.56%；赋予AVM优异的抗紫外光分解性能，强紫外光照射60min后，由AVM水乳液中AVM的残留率14.03%提高到DA/CMC-g-PMMA@AVM中的59.55%。载药微胶囊中药物释放具有pH响应，在pH=5条件下出现爆释，药物释放过程符合Weibull模型，受Fick扩散控制。

关键词: 载体, 多巴胺, 阿维菌素, 叶面亲和, 稳定性, 可持续性

Abstract:

In order to reduce the loss of pesticides, a foliar affinity sustained-release microcapsules was designed. Polymethyl methacrylate (PMMA) was used to modify carboxymethyl cellulose (CMC), and then avermectin (AVM) was coated by self-assembly to form drug-loaded microcapsules (CMC-g-PMMA@AVM). The dopamine coating was then used to form affinity microcapsules (DA/CMC-g-PMMA@AVM). The structure and morphology were characterized by scanning electron microscopy, infrared spectroscopy and thermogravimetric analysis. The drug loading, leaf surface wetting and pH-responsive drug release properties were studied. The results showed that DA/CMC-g-PMMA@AVM was a spherical particle with an average particle size of 126nm. The coating of dopamine can effectively improve the drug loading performance of the microsphere and increase the encapsulation efficiency to 88.56%. The leaf affinity of AVM was enhanced and the leaf retention was increased by 30.56% relative to the emulsion of avermectin. The residual rate of AVM in AVM emulsion was only 14.03% after strong ultraviolet irradiation for 60min, while up to 59.55% in DA/CMC-g-PMMA@AVM. The drug release in the microcapsules had a pH response, and a burst release phenomenon occurred at pH=5. The release process conformd to the Weibull model and was controlled by Fick diffusion.

Key words: support, dopamine, avermectin, foliar affinity, stability, sustainability

中图分类号:

TQ314

陈龙,周红军,江海科,郝丽,陈铧耀,周新华. 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.

Long CHEN,Hongjun ZHOU,Haike JIANG,Li HAO,Huayao CHEN,Xinhua ZHOU. Preparation and pH responsive release properties of foliar affinity avermectin microcapsules[J]. Chemical Industry and Engineering Progress, 2020, 39(1): 348-355.

图/表 11

图1 CMC-g-PMMA的合成机理

图2 红外光谱图a—CMC； b—DA； c—CMC-g-PMMA；d—DA/CMC-g-PMMA@AVM； e—AVM

图3 CMC和CMC-g-PMMA的TG和DTG图

图4 CMC-g-PMMA、CMC-g-PMMA@AVM和DA/CMC-g-PMMA@AVM的扫描电镜图及其粒径分布图

表1 不同DA添加量对包封率的影响

样品	DA/g	EE/%
CMC-g-PMMA@AVM	0	73.35
DA-0.05/CMC-g-PMMA@AVM	0.05	83.89
DA-0.10/CMC-g-PMMA@AVM	0.10	84.35
DA-0.15/CMC-g-PMMA@AVM	0.15	88.56

图5 样品在黄瓜叶面的接触角

图6 AVM水乳液、CMC-g-PMMA@AVM与DA/CMC-g-PMMA@AVM的叶面滞留量

图7 不同条件下制备的DA/CMC-g-PMMA@AVM在不同AVM浓度下的表面张力

图8 紫外照射下AVM溶液、CMC-g-PMMA@AVM和DA/CMC-g-PMMA@AVM中AVM的残留率

图9 DA/CMC-g-PMMA@AVM在不同pH条件下AVM的释放曲线及zeta电位的变化

表2 模型拟合结果

模型	方程	pH	a₀	a₁	R²
Zero-order	y=a₀x	3	0.0089	—	0.7123
		5	0.0102	—	0.5419
		7	0.0085	—	0.7294
		9	0.0086	—	0.7707
First-order	y=a₀[1－exp(-a₁x)]	3	0.8596	0.0857	0.9056
		5	0.9639	0.2814	0.9796
		7	0.8276	0.0726	0.8564
		9	0.8734	0.0527	0.9125
Weibull model	y=1－exp(-x^a⁰/a₁)	3	0.5128	4.7199	0.9942
		5	0.6922	2.7166	0.9964
		7	0.4756	4.8366	0.9748
		9	0.5653	6.7972	0.9829
Higuchi model	y=a₀x^0.5	3	0.0985	—	0.7795
		5	0.1201	—	0.1931
		7	0.0929	—	0.7943
		9	0.0927	—	0.8919

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