摘要
基于分子间相互作用筛选了对新烟碱类农药分子有强亲和力的卟吩基金属有机框架材料(MOF)配体。新烟碱类农药分子与中-四(4-羧基苯基)卟吩(H4TCPP)配体主要通过π-π相互作用、CH···π和Cl···π等弱相互作用结合。以八水合氯氧化锆、中-四(4-羧基苯基)卟吩和苯甲酸为原料采用溶剂热法制备了MOF-525,再通过聚乙烯醇(PVA)将MOF-525固定在三聚氰胺海绵(MS)上得到MOF-525复合三聚氰胺海绵(MOF-525@MS)。使用扫描电子显微镜(SEM)、能量色散X射线光谱(XPS)、X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)和热重分析(TG)多种方法对MOF-525@MS的结构进行了表征。将MOF-525@MS作为吸附剂对水中4种新烟碱类农药(烯啶虫胺、噻虫嗪、啶虫脒和吡虫啉)进行吸附实验条件优化、实际样品测定和可重复利用性测定。结果表明,pH=5、吸附时间15 min和NaCl质量分数为8%是MOF-525@MS对4种新烟碱农药的最佳吸附去除条件。取黄浦江水、田间水和湖水3种水样进行不同浓度的农药加标(100、200和300 mg/L),MOF-525@MS在这3种水样中对农药均有80.61%~97.82%的去除率。最后,经过吸附-洗脱-干燥-再吸附重复5个循环后MOF-525@MS的去除率仍有75.41%~81.20%,具有较好的可重复利用性,是可用于水中新烟碱类农药去除的良好吸附材料。
Porphyrin based-metal organic framework(MOF)with strong affinity for neonicotinoid pesticide molecules were screened based on intermolecular interactions.Neonicotinoid pesticide molecules bind to meso-tetrakis(4-carboxyphenyl)porphyrin(H4TCPP)ligands mainly through weak interactions such asπ-πinteractions,CH…πand Cl…π.MOF-525 was prepared by solvothermal method using zirconium chloride octahydrate,meso-tetra(4-carboxyphenyl)porphin,and benzoic acid as the raw materials.MOF-525 was immobilized on a melamine sponge(MS)by poly(vinyl alcohol)(PVA)to obtain MOF-525 composite melamine sponge(MOF-525@MS).The structure of MOF-525@MS was characterized by using scanning electron microscopy(SEM),energy dispersive X-ray spectroscopy(EDS),X-ray diffraction(XRD),Fourier-transform infrared spectroscopy(FT-IR),and thermogravimetric(TG),respectively.MOF-525@MS was used as an adsorbent for the optimization of adsorption experimental conditions,determination of actual samples and determination of reusability of four neonicotinoid pesticides(nitenpyram,thiamethoxam,acetamiprid and imidacloprid)in water.The results showed that the removal rate of MOF-525@MS for the above four neonicotinoid pesticides was over 87.49%at pH=5,adsorption time of 15 min and 8%NaCl.Three kinds of water samples from Huangpu River,field water and lake water were spiked with different concentrations of pesticides(100,200 and 300 mg/L),and MOF-525@MS showed 80.61%~97.82%removal of pesticides in all three kinds of water samples.Finally,the removal rate was still 75.41%~81.20%after five cycles of adsorption-elution-drying-re-adsorption repetition,which has good reusability and is a good adsorbent material that can be used for the removal of neonicotinoid pesticides in water.
作者
张馨煜
黄剑辉
黄磊
张大铭
徐斐
吴秀秀
ZHANG Xin-Yu;HUANG Jian-Hui;HUANG Lei;ZHANG Da-Ming;XU Fei;WU Xiu-Xiu(School of Health Science and Engineering,University of Shanghai for Science and Technology,Shanghai 200093,China;Shanghai Engineering Research Center of Food Rapid Detection,Shanghai 200093,China;Shanghai Ruixin Technology Instrument Co.,Ltd.,Shanghai 200331,China)
出处
《应用化学》
北大核心
2025年第8期1144-1154,共11页
Chinese Journal of Applied Chemistry
基金
上海市优秀学术/技术带头人计划项目(No.22XD1434700)
国家自然科学基金(No.32302219)资助。
关键词
金属有机框架
复合材料
新烟碱类农药
吸附性去除
Metal-organic framework
Composite materials
Neonicotinoid pesticides
Adsorptive removal
作者简介
吴秀秀,E-mail:xiuxiuwu@usst.edu.cn。
