镁改性硅藻土对苦参碱的吸附释放性能研究

doi:10.19964/j.issn.1006-4990.2022-0757

Abstract

Abstract:

The overuse of chemical pesticides has caused serious environmental problems. Using plant source pesticides is a new way to control pests and reduce agricultural residues.However，the short effect and easy degradation limit its wide application.The magnesium oxide modified diatomite（MD） was used as a drug carrier，which could form a complex with the plant derived pesticide matrine and make it adhere to the surface of MD.Magnesium oxide modified diatomite was characterized by specific surface area analyzer，scanning electron microscope and energy spectrum，and the preparation process，adsorption mechanism and slow release properties were discussed.The study showed that the magnesium oxide modified diatomite had more adsorption sites.Compared with the original diatomite，the adsorption capacity of the magnesium oxide modified diatcomite for matrine was increased by 130%.The adsorption kinetics and thermodynamics showed that the adsorption of matrine on magnesium oxide modified diatomite was more consistent with the Freundlich adsorption model and the quasi-second-order kinetic model.It was revealed that the adsorption was a chemical endothermic process of polymolecular adsorption.The release kinetics study indicated that the release process was mainly controlled by Fick diffusion.The release time was prolonged from 4 h to 180 h compared with that of commercially available liposomes and protein microcapsules.This study explored the preparation process and sustained-release performance of diatomite based plant-derived sustained-release pesticides，which could provide theoretical reference for actual drug use in the field.

Key words: matrine, diatomite, adsorption, sustained release performance, kinetics

CLC Number:

X384

DING Ning, ZHANG Jian, PING Qingwei, SHENG Xueru, LI Na. Study on adsorption and release properties of matrine by magnesium-modified diatomite[J]. Inorganic Chemicals Industry, 2023, 55(11): 37-46.

Figures/Tables 14

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References 30

1	陈锋，孟顺龙，陈家长.农药在沉积物-水-生物体的污染特征综述［J］.中国农学通报，2021，37（7）：159-164.
	CHEN Feng， MENG Shunlong， CHEN Jiachang.Pollution status of pesticides in water-sediment-organisms：A review［J］.Chinese Agricultural Science Bulletin，2021，37（7）：159-164.
2	YAN Shuo， HU Qian， JIANG Qinhong，et al.Simple osthole/nanocarrier pesticide efficiently controls both pests and diseases fulfilling the need of green production of strawberry［J］.ACS Applied Materials & Interfaces，2021，13（30）：36350-36360.
3	袁昳雯.绿色食品稻谷生产中农药使用及最大残留限量标准比对分析［J］.上海农业科技，2022（4）：33-38，72.
	YUAN Yiwen.Comparative analysis of pesticide use and maximum residue limit standards in green food rice production［J］.Shanghai Agricultural Science and Technology，2022（4）：33-38，72.
4	杨欣蕊，廖艳凤，赵鹏飞，等.植物源农药及其开发利用研究进展［J］.南方农业，2022，16（11）：33-36.
	YANG Xinrui， LIAO Yanfeng， ZHAO Pengfei，et al.Study progress in plant-source pesticides and their development and utilization［J］.South China Agriculture，2022，16（11）：33-36.
5	于忻滢，张国良，范松，等.植物源农药研究进展［J］.黑龙江农业科学，2021（7）：123-129.
	YU Xinying， ZHANG Guoliang， FAN Song，et al.Research progress of botanical pesticides［J］.Heilongjiang Agricultural Sciences， 2021（7）：123-129.
6	李结瑶，罗文翰，黎汉清，等.农药微胶囊壁材设计研究进展［J］.包装工程，2023，44（1）：52-60.
	LI Jieyao， LUO Wenhan， LI Hanqing，et al.Research progress on design of pesticide microcapsule wall［J］.Packaging Engineering，2023，44（1）：52-60.
7	时海涛，徐勇，张泗达，等.天然源材料在农药剂型加工中的研究进展［J］.中国植保导刊，2022，42（8）：20-23，36.
	SHI Haitao， XU Yong， ZHANG Sida，et al.Research progress in the use of natural source materials for pesticide formulation［J］.China Plant Protection，2022，42（8）：20-23，36.
8	DU Yu， ZHANG Qizhen， YU Manli，et al.Sodium alginate-based composite microspheres for controlled release of pesticides and reduction of adverse effects of copper in agricultural soils［J］.Chemosphere，2023，313：137539.
9	张晋天，张慧学，马忠华，等.缓/控释农药研究及其应用进展［J］.湖南师范大学自然科学学报，2022，45（5）：117-123.
	ZHANG Jintian， ZHANG Huixue， MA Zhonghua，et al.Progress and application of slow/controlled release of pesticides［J］.Journal of Natural Science of Hunan Normal University，2022，45（5）：117-123.
10	吴相川，任雪云.硅藻土理化特性及改性研究［J］.西部皮革，2016，38（14）：34.
	WU Xiangchuan， REN Xueyun.Study on physical and chemical properties and modification of diatomite［J］.West Leather，2016，38（14）：34.
11	张育新，戴兴健，张臣智，等.硅藻土特性、提纯及在生物医药领域中的应用［J］.矿产保护与利用，2021，41（6）：46-56.
	ZHANG Yuxin， DAI Xingjian， ZHANG Chenzhi，et al.Research progress on the properties of diatomite and its application in biomedical field［J］.Conservation and Utilization of Mineral Resour-ces，2021，41（6）：46-56.
12	张育新，丁杰航，鄢文磊，等.硅藻土基硅肥的研究进展［J］.矿产保护与利用，2022，42（4）：85-93.
	ZHANG Yuxin， DING Jiehang， YAN Wenlei，et al.Recent advances of diatomite-based silicon fertilizer［J］.Conservation and Utilization of Mineral Resources，2022，42（4）：85-93.
13	LI Chunyan， SHENG Xueru， LI Na，et al.Insecticidal characteristics and mechanism of a promising natural insecticide against saw-toothed grain beetle［J］.RSC Advances，2022，12（12）：7066-7074.
14	杨勤桃，解庆林，陈南春.壳聚糖改性硅藻土对水中As（Ⅴ）的吸附特性［J］.非金属矿，2021，44（5）：103-106.
	YANG Qintao， XIE Qinglin， CHEN Nanchun.Adsorption behaviors of As（Ⅴ） in water by chitomite-modified diatomite［J］.Non-Metallic Mines，2021，44（5）：103-106.
15	范艺，王哲，赵连勤，等.锆改性硅藻土吸附水中磷的研究［J］.环境科学，2017，38（4）：1490-1496.
	FAN Yi， WANG Zhe， ZHAO Lianqin，et al.Modification of diatomite by zirconium and its performance in phosphate removal from water［J］.Environmental Science，2017，38（4）：1490-1496.
16	吴盈秋，夏鹏，李远，等.镁改性硅藻土回收废水氮磷产物对水中Pb²⁺和Zn²⁺的去除［J］.环境科学，2022，43（12）：5667-5675.
	WU Yingqiu， XIA Peng， LI Yuan，et al.Removal of Pb（Ⅱ） and Zn（Ⅱ） from wastewater via magnesium-modified diatomite product recovering nitrogen and phosphorus［J］.Environmental Science，2022，43（12）：5667-5675.
17	LIU Ying， ZHANG Jian， SHENG Xueru，et al.Adsorption and release kinetics，equilibrium，and thermodynamic studies of hymexazol onto diatomite［J］.ACS Omega，2020，5（45）：29504-29512.
18	XIA Peng， WANG Xuejiang， WANG Xin，et al.Synthesis and characterization of MgO modified diatomite for phosphorus recovery in eutrophic water［J］.Journal of Chemical & Engineering Data，2017，62（1）：226-235.
19	TAYLOR R， KENNARD O， VERSICHEL W.Geometry of the imino-carbonyl（N-H...O：C） hydrogen bond.1.Lone-pair directionality［J］.Journal of the American Chemical Society，1983，105（18）：5761-5766.
20	程圆杰，郭雯婷，崔蕊蕊，等.苦参碱水解与水中降解研究［J］.山东工业技术，2019（6）：68.
	CHENG Yuanjie， GUO Wenting， CUI Ruirui，et al.Study on hydrolysis and degradation of matrine in water［J］.Shandong Industrial Technology，2019（6）：68.
21	徐荣声，冯倩，孟泽，等.枸杞杆制活性炭对亚甲基蓝的吸附研究［J］.无机盐工业，2022，54（12）：106-112，118.
	XU Rongsheng， FENG Qian， MENG Ze，et al.Study on adsorption of methylene blue by activated carbon prepared by wolfberry stems［J］.Inorganic Chemicals Industry，2022，54（12）：106-112，118.
22	袁新华，刘敦舜，刘怡，等.苦参碱分子印迹氢键型超高交联吸附树脂的制备及吸附性能［J］.江苏大学学报（自然科学版），2019，40（5）：585-590.
	YUAN Xinhua， LIU Dunshun， LIU Yi，et al.Preparation and adsorption properties of hydrogen-bonded molecular imprinting hypercrosslinked polymeric adsorbent for Matrine［J］.Journal of Jiangsu University（Natural Science Edition），2019，40（5）：585- 590.
23	CHEN Haohao， LUO Shaojian， ZHENG Xikang，et al.Separation of matrine and oxymatrine from Sophora flavescens extract through cation exchange resin coupled with macroporous absorption resin［J］.Polish Journal of Chemical Technology，2016，18（2）：31-39.
24	TIAN Peng， HAN Xiuying， NING Guiling，et al.Synthesis of porous hierarchical MgO and its superb adsorption properties［J］.ACS Applied Materials & Interfaces，2013，5（23）：12411-12418.
25	ROUQUEROL F， ROUQUEROL J， SING K S W，et al.Introduction［M］//Adsorption by Powders and Porous Solids.Amsterdam：Elsevier，2014：1-24.
26	INGLEZAKIS V J， POULOPOULOS S G.Inglezakis.Adsorption，ion exchange and catalysis［M］.Greece：Elsevier，2006：31-56.
27	秦庆东.介孔硅材料吸附水中污染物技术与原理［M］.南京：东南大学出版社，2015：10-25.
28	KARIMI ALAVIJEH R， AKHBARI K.Biocompatible MIL-101（Fe） as a smart carrier with high loading potential and sustained release of curcumin［J］.Inorganic Chemistry，2020，59（6）：3570-3578.
29	ALMEIDA C M R， GHICA M E， DURÃES L.An overview on alumina-silica-based aerogels［J］.Advances in Colloid and Interface Science，2020，282：102189.
30	马志卿，豆敏详，姚满，等.苦参碱的水解动态及其在自然水体中的降解特性［J］.农药学学报，2017，19（3）：347-354.
	MA Zhiqing， DOU Minxiang， YAO Man，et al.Hydrolysis dynamic of matrine and its degradation properties in natural waters［J］.Chinese Journal of Pesticide Science，2017，19（3）：347-354.

温度/℃	∆G/（kJ∙mol^-1）	∆H/（kJ∙mol^-1）	∆S/（kJ∙mol^-1）
30	-40.439	-21.047	0.064
40	-41.039	-21.047	0.064
50	-41.719	-21.047	0.064

温度/℃	Langmuir模型			Freundlich模型
温度/℃	Q_max	K_L	R²	K_F	1/n	R²
30	35.198	0.011	0.627 5	0.937	0.826	0.963
40	25.102	0.030	0.928 3	1.233	0.648	0.991
50	28.826	0.034	0.938 4	0.689	0.661	0.988

温度/℃	准一级动力学模型			准二级动力学模型				Elovich方程模型			颗粒内扩散模型
温度/℃	Q_e	K₁	R²	Q_e	K₂	R²		α	β	R²	K	C	R²
30	0.157	0.440	0.806	0.408	2.508	0.997	0.028		0.304	0.890	0.018	0.307	0.955
40	0.039	0.277	0.871	0.385	7.669	0.999	0.010		0.384	0.864	0.006	0.349	0.940
50	0.044	0.372	0.861	0.388	8.356	0.999	0.010		0.352	0.965	0.006	0.335	0.996

pH	零级动力学模型		一级动力学模型			Ritger-Peppas模型
pH	K₀	R²	K₁	R²		n	log K₂	R²
6	0.065	0.938	-8.805	0.700	0.190		-0.920	0.919
7	0.124	0.911	-0.001	0.934	0.264		-0.964	0.995
8	0.113	0.687	-0.001	0.934	0.251		-0.985	0.973

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Study on adsorption and release properties of matrine by magnesium-modified diatomite

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