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基于多孔碳酸钙构建的双pH响应性嘧菌酯控释微球的制备及其生物安全性

徐鹏 王澳 黄刚 韩媛如 石伟山 邢刚 唐蜜 包佳伟

徐鹏, 王澳, 黄刚, 等. 基于多孔碳酸钙构建的双pH响应性嘧菌酯控释微球的制备及其生物安全性[J]. 复合材料学报, 2024, 42(0): 1-10.
引用本文: 徐鹏, 王澳, 黄刚, 等. 基于多孔碳酸钙构建的双pH响应性嘧菌酯控释微球的制备及其生物安全性[J]. 复合材料学报, 2024, 42(0): 1-10.
XU Peng, WANG Ao, HUANG Gang, et al. Dual pH responsive azoxystrobin controlled release microspheres constructed from porous calcium carbonate and its biosecurity[J]. Acta Materiae Compositae Sinica.
Citation: XU Peng, WANG Ao, HUANG Gang, et al. Dual pH responsive azoxystrobin controlled release microspheres constructed from porous calcium carbonate and its biosecurity[J]. Acta Materiae Compositae Sinica.

基于多孔碳酸钙构建的双pH响应性嘧菌酯控释微球的制备及其生物安全性

基金项目: 江苏省林业科技创新与推广项目(LYKJ-南京[2022]02)
详细信息
    通讯作者:

    徐鹏,博士,副教授,硕士生导师,研究方向为纳米农药开发与应用 E-mail: xupeng@njfu.edu.cn

  • 中图分类号: TB333

Dual pH responsive azoxystrobin controlled release microspheres constructed from porous calcium carbonate and its biosecurity

Funds: Jiangsu Forestry Science and Technology Innovation and Promotion Project (LYKJ-Nanjing[2022]02)
  • 摘要: 刺激响应性农药控释系统为提高农药利用效率和减少环境污染提供了强有力的策略。本研究中,在采用共沉淀法制备多孔碳酸钙微球(CaCO3)的基础上,通过浸渍吸附法获得负载嘧菌酯(Az)的多孔碳酸钙微球(Az/CaCO3),并在复合微球表面进一步包覆单宁酸-Cu2+络合物,构建了一个具有双pH响应性的嘧菌酯控释系统(Az/CaCO3@TA-Cu)。理化性能研究表明成功制备了Az/CaCO3@TA-Cu微球,其载药量为16.42%。模拟释放研究结果表明Az/CaCO3@TA-Cu具有良好的pH控释性能,在pH=7的磷酸缓冲溶液中96 h累积释放率为36.99%,而在pH=5和pH=9条件下的累积释放率分别为74.32%和58.79%。菌丝体生长速率实验表明Az/CaCO3@TA-Cu对禾谷镰刀菌生长具有较好的抑制作用,中值抑制浓度为纯Az和Az/CaCO3的6.58倍和3.28倍。此外,小麦发芽率和斑马鱼存活率统计结果显示,Az/CaCO3@TA-Cu相对于Az/CaCO3和纯Az表现出更优的生物安全性。

     

  • 图  1  CaCO3(a)和单宁酸包覆的嘧菌酯/多孔CaCO3载药系统(Az/CaCO3@TA-Cu)(b)的SEM图,及Az/CaCO3@TA-Cu中的O、Ca、Cl和Cu元素映射图(c)

    Figure  1.  SEM images of CaCO3 (a) and tannic acid-coated pyrimethanil/porous CaCO3 carrier system (Az/CaCO3@TA-Cu) (b), elemental mapping of O, Ca, Cl and Cu in Az/CaCO3@TA-Cu (c)

    图  2  Az、CaCO3、Az/CaCO3、Az/CaCO3@TA-Cu的电位图(a)和红外吸收光谱图(b)

    Figure  2.  Potentials (a) and FT-IR (b) of Az、CaCO3、Az/CaCO3、Az/CaCO3@TA-Cu

    图  3  Az、Az/CaCO3、Az/CaCO3@TA-Cu的TG曲线(a)和在土壤中的释放曲线(b)

    Figure  3.  TG curves of Az、Az/CaCO3、Az/CaCO3@TA-Cu (a) and release curves in soil (b)

    图  4  Az/CaCO3和Az/CaCO3@TA-Cu中Az的释放曲线(a); 不同pH条件下 Az/CaCO3@TA-Cu的释放曲线(b)

    Figure  4.  Release curves of Az in Az/CaCO3 and Az/CaCO3@TA-Cu (a); Release curves Az/CaCO3@TA-Cu under different pH conditions (b)

    图  5  使用零级方程(a); 一级方程(b); Higuchi方程(c); Ritger-Peppas方程(d)拟合Az/CaCO3@TA-Cu在不同pH条件下的曲线

    Figure  5.  Fitting of Az/CaCO3@TA-Cu curves at different pH conditions using zero-order equations (a); first-order equations (b); Higuchi's equation (c); Ritger-Peppas' equation (d)

    图  6  Az、Az/CaCO3和Az/CaCO3@TA-Cu在不同浓度下,对禾谷镰刀菌病在第 3-5 天的抑菌情况

    Figure  6.  Inhibition of Fusarium graminearum disease by Az、Az/CaCO3 and Az/CaCO3@TA-Cu at different concentrations at day 3-5

    图  7  Az、Az/CaCO3和Az/CaCO3@TA-Cu在不同浓度下,对小麦发芽的影响

    Figure  7.  Effect of Az, Az/CaCO3 and Az/CaCO3@TA-Cu at different concentrations on germination of wheat

    图  8  Az、Az/CaCO3和Az/CaCO3@TA-Cu在不同浓度下,对斑马鱼的影响

    Figure  8.  Effects of Az, Az/CaCO3 and Az/CaCO3@TA-Cu at different concentrations on zebrafish

    表  1  通过拟合几个动力学方程计算Az/CaCO3@TA-Cu释放Az的参数

    Table  1.   Parameters for Az/CaCO3@TA-Cu release of Az by fitting several kinetic equations

    Model pH values k n r2
    Zero-order 5 0.555 0.618
    7 0.448 0.572
    9 0.294 0.740
    First-order 5 0.159 0.895
    7 0.130 0.813
    9 0.155 0.963
    Higuchi 5 6.570 0.851
    7 3.237 0.921
    9 5.397 0.820
    Ritger-Peppas 5 28.416 0.226 0.978
    7 11.815 0.259 0.991
    9 21.980 0.235 0.951
    Notes: k is the release rate constant; n is the release characteristic index; r 2 is the regression coefficient.
    下载: 导出CSV

    表  2  禾谷镰刀菌病原菌抗真菌活性测试结果

    Table  2.   Results of antifungal activity test of Fusarium graminearum pathogens

    Day 3
    Sample Toxicity regression equation EC50 /
    (mg·L−1)
    Standard error R2
    Pure Az y=0.339x-0.4266 18.19 0.140 0.9696
    Az/CaCO3 y=0.394x-0.3035 5.77 0.138 0.9592
    Az/CaCO3@TA-Cu y=0.475x-0.1310 1.88 0.136 0.9776
    Day 4
    Sample Toxicity regression equation EC50/
    (mg·L−1)
    Standard error R2
    Pure Az y=0.468x-0.4708 11.41 0.145 0.9040
    Az/CaCO3 y=0.439x-0.3869 7.87 0.141 0.9608
    Az/CaCO3@TA-Cu y=0.526x-0.2334 2.79 0.140 0.9042
    Day 5
    Sample Toxicity regression equation EC50/
    (mg·L−1)
    Standard error R2
    Pure Az y=0.447x-0.6147 18.40 0.150 0.9648
    Az/CaCO3 y=0.556x-0.4176 5.61 0.145 0.9977
    Az/CaCO3@TA-Cu y=0.558x-0.245 2.80 0.140 0.9361
    Notes: EC50 is median effect concentration; R2 is the regression coefficient.
    下载: 导出CSV
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  • 收稿日期:  2024-04-26
  • 修回日期:  2024-05-24
  • 录用日期:  2024-05-31
  • 网络出版日期:  2024-06-26

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