本文關鍵詞：表面活性劑修飾磁性納米材料及其在環(huán)境有機污染物分析中的應用　出處：《蘇州科技大學》2017年碩士論文　論文類型：學位論文

  更多相關文章： 有機污染物 苯脲類除草劑 磁性固相萃取 表面活性劑 超聲萃取 超高效液相色譜-質譜

【摘要】：磁性固相萃取作為一種新型的前處理方式在環(huán)境監(jiān)測領域已經得到了廣泛的應用,其核心組成部分是磁性吸附材料,但是商品化的磁性材料合成條件較為苛刻,且價格過于昂貴,實驗成本較高。通過實驗室自制的磁性材料作為磁性固相萃取的吸附劑,不僅合成步驟較為簡單,也可大大降低實驗成本。本文主要是通過實驗室自制的磁性納米材料,并用表面活性劑對其修飾,將修飾后的磁性材料用作磁性固相萃取中的吸附劑對水樣和土壤樣品中常見的四種苯脲類有機污染物(滅草隆、敵草隆、綠麥隆、異丙隆)進行測定,主要研究內容:(1)磁性吸附劑的合成:采用經典的共沉淀法,在堿性條件下通過優(yōu)化滴加氨水的時間來合成磁性納米粒子(Fe_3O_4MNPs)。將合成的Fe_3O_4MNPs先用SiO_2修飾,以減少Fe_3O_4MNPs的團聚現(xiàn)象,再用十二烷基硫酸鈉(SDS)修飾,使Fe_3O_4MNPs表面具有吸附化合物的孔穴。通過優(yōu)化SiO_2以及SDS的用量,使得所制備的磁性材料粒徑更小,分散性更好。將合成的磁性材料進行掃描電鏡和傅里葉紅外表征。合成出的磁性材料表面具有很多的孔穴,對待測物質具有吸附性。(2)用實驗室自制的磁性材料作為磁性固相萃取中的吸附劑,并結合超高效液相色譜-質譜法測定水樣中的四種苯脲類化合物,并與商品化的磁性材料進行了對比。考察了活化溶劑種類及用量、磁性材料的種類及用量、pH、酸的種類、洗脫溶劑的種類及體積、振蕩時間等因素對四種苯脲類除草劑回收率的影響。確定最佳優(yōu)化條件為:50m L的水樣用鹽酸調節(jié)到pH=5,活化溶劑為5m L的乙腈,80KHz超聲分散3min,磁性吸附劑的用量為70mg,洗脫溶劑為4m L乙腈,振蕩15min,四種待測物質的加標回收率在86.2%-95.4%之間。方法的線性范圍是0.05-5.0μg/L,相關性系數(shù)都大于0.999,相對標準偏差3.0-6.6%,方法檢出限(LOD)范圍為10.9-13.3ng/L。用乙腈浸泡磁性材料,然后低溫烘干后重復利用。磁性材料經過多次的重復使用,未見待測物質的回收率有明顯下降趨勢。該方法具有快速、靈敏、磁性材料可重復使用且減少分析過程中有機試劑對環(huán)境污染等優(yōu)點。(3)采用超聲提取法先提取土壤中的四種苯脲類物質,將提取液氮吹近干后加入水稀釋復溶,將磁性固相萃取法用作土壤中待測物的凈化技術,建立了土壤中四種苯脲類除草劑的前處理方法,并采用超高效液相色譜質譜法進行定性定量分析。并將磁性固相萃取法與固相萃取法進行了對比�？疾炝溯腿∪軇�、超聲頻率、萃取時間、初始超聲萃取溫度、稀釋水樣體積、磁性納米材料的用量、振蕩時間、洗脫溶劑的體積對土壤中待測物質回收率的影響。最佳萃取條件是:10m L乙醇在80KHz條件下超聲15min,初始超聲溫度為40℃。凈化條件是:150m L的稀釋水樣,100mg的磁性吸附材料,25min振蕩時間,6m L乙腈洗脫�；厥章试�79.8~85.2%之間,方法的線性范圍是5-200μg/kg,相關性系數(shù)都大于0.995,相對標準偏差4.6-7.9%,方法檢出限(LOD)范圍為0.2-0.7μg/kg,該方法具有操作簡便,檢出限低,靈敏度高等特點,適用于土壤中痕量苯脲類物質的測定。
[Abstract]:Magnetic solid phase extraction as a new pretreatment method has been widely used in the field of environmental monitoring, the core part is the magnetic adsorption materials, magnetic materials but commercial synthesis conditions are harsh, and the price is too expensive, the high cost of experiment. Through the self-made magnetic material as magnetic adsorbents for solid-phase extraction not only, the synthesis step is relatively simple, but also can greatly reduce the experimental cost. This paper is mainly through the self-made magnetic nano materials, and surfactant on the modification, the magnetic material of modified magnetic solid phase extraction as adsorption agent on water and soil samples of four kinds of common phenylureas organic pollutants (monuron and diuron and Chlortoluron and isoproturon) were determined. The main research contents are as follows: (1) the synthesis of magnetic adsorbents by co precipitation method in the classic, alkaline conditions Under the optimized by adding ammonia time to synthesis of magnetic nanoparticles (Fe_3O_4MNPs). The first synthesis of Fe_3O_4MNPs modified with SiO_2, in order to reduce the agglomeration of Fe_3O_4MNPs, with twelve sodium dodecyl sulfate (SDS) modification of the Fe_3O_4MNPs surface hole with adsorption compounds. Through the optimization of SiO_2 and the amount of SDS, makes the magnetic the material with smaller size particle preparation, better dispersion. The magnetic material is synthesized by scanning electron microscopy and Fourier transform infrared spectra. The synthesized magnetic material surface has many holes, measured with adsorption material. (2) with self-made magnetic materials as adsorbent magnetic solid phase extraction, and determination of four phenylurea compounds in water using ultra high performance liquid chromatography-mass spectrometry, compared with commercial and magnetic materials. The effect of activation of solvent type and amount, the kind of magnetic material Type and dosage, pH, acid type, type and volume of elution solvent. The effect of oscillation time and other factors on four herbicides recovery. Determine the best optimized condition is: 50m L water sample with hydrochloric acid to adjust to pH=5, activation of acetonitrile solvent for L 5m, 80KHz 3min, ultrasonic dispersion, magnetic adsorption the dosage is 70mg, elution solvent is 4m L acetonitrile, 15min four kinds of oscillation, the recovery rate of the substance to be tested in 86.2%-95.4%. The linear range is 0.05-5.0 ~ g/L, the correlation coefficient is greater than 0.999, the relative standard deviation is 3.0-6.6%, the detection limit of the method (LOD) with acetonitrile immersion magnetic materials for 10.9-13.3ng/L. then, low temperature drying after repeated use of magnetic materials. After used repeatedly, no analyte recovery rate decreased significantly. The method is rapid, sensitive, magnetic materials can be reused and reduced in the process of organic analysis Reagents on environmental pollution and other advantages. (3) extract in soil four phenylurea compounds extracted by ultrasonic extraction method, adding water blown nearly dry after liquid nitrogen dilution solution, the magnetic solid phase extraction method for the purification technology of soil analytes, established a pretreatment method of four phenylureas the herbicide in the soil, and the use of mass spectrometry UPLC qualitative and quantitative analysis. Comparing the magnetic solid phase extraction and solid-phase extraction method. The effects of extraction solvent, extraction time, ultrasonic frequency, ultrasonic extraction and initial temperature, dilution water volume, magnetic nano material dosage, oscillation time, elution solvent the volume of soil to be measured in the material recovery rate. The best extraction conditions are: 10M L 80KHz 15min in ethanol ultrasonic conditions, initial temperature of 40 DEG. Ultrasonic purification conditions are: dilution water 150m L, magnetic adsorbent 100mg, 2 5min 6m L oscillation time, acetonitrile. The recovery rate was 79.8~85.2%, the linear range is 5-200 ~ g/kg, the correlation coefficient is greater than 0.995, the relative standard deviation is 4.6-7.9%, the detection limit of the method (LOD) is in the range of 0.2-0.7 g/kg, this method has the advantages of simple operation, low detection limit, high sensitivity, suitable for determination of soil trace phenylurea compounds.

【學位授予單位】：蘇州科技大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：X830;TB383.1

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