本文關鍵詞：鉛印跡介孔硅材料和CdSe量子點的制備及在鉛離子分離檢測中的應用　出處：《上海師范大學》2017年碩士論文　論文類型：學位論文

  更多相關文章： 鉛離子印跡介孔硅材料 選擇性吸附 硒化鎘量子點 電致化學發(fā)光 鉛離子

【摘要】：鉛離子廣泛存在于環(huán)境中,因其毒害性和在生物體中的可積累性,對人體和生物體構成了嚴重的威脅。目前,已用于實際的檢測鉛離子的方法往往具有前處理復雜、檢出限高、選擇性差等問題。因此,建立可靠、高靈敏、高選擇性的分離和檢測鉛離子的方法具有重要意義。本論文制備了兩種類型的功能化納米材料:雙吡唑基團功能化的鉛離子印跡介孔硅材料和具有光學性質(zhì)的巰基丙酸包被的硒化鎘量子點(Cd Se QDs)。將功能化介孔硅材料用作固相萃取填充劑來選擇性分離鉛離子,并與電感耦合等離子體質(zhì)譜(inductively coupled plasma-atomic mass spectrometry,ICP-MS)聯(lián)用,實現(xiàn)了對水中鉛離子分離與檢測。其次,初步構建了基于Cd Se量子點的液相電致化學發(fā)光(electrochemiluminescence,ECL)檢測鉛離子的方法。詳細工作包括以下三個方面的內(nèi)容:1.設計并合成了三種含氮雙齒配體修飾的鉛離子印跡介孔硅材料。印跡材料均以4-(二(1-氫吡唑))甲基苯酚作為功能單體,鉛離子為模板,3-異氰酸丙基三乙氧基硅烷為交聯(lián)劑,不同形貌特征的介孔硅材料SBA-15、MCM-41和FDU-12分別做為固相載體,采用表面印跡技術,經(jīng)模板洗脫后分別得到Pb-IIMS-SBA-15、Pb-IIMS-MCM-41和Pb-IIMS-FDU-12印跡介孔材料。經(jīng)紅外光譜、固態(tài)硅譜和碳譜的分析證明了功能單體已成功修飾于介孔材料表面;掃描電鏡、透射電鏡、X射線小角衍射和氮氣吸附脫附等表征證明所得材料均保持原有介孔硅的形貌特征。通過能量色散X射線元素分析表明Pb-IIMS-MCM-41具有最高的含氮量。此外,三種相應的非印跡材料也成功制備。2.鉛離子印跡介孔硅材料吸附性能的研究及其在水樣分析中的應用。對鉛印跡材料及相應的非印跡材料吸附量和選擇性進行了考察,結果表明經(jīng)印跡后的介孔硅材料在對鉛離子的吸附量和選擇性上確實均有明顯的提高。吸附等溫線和吸附動力學實驗表明三種印跡材料對鉛離子均具有較大的吸附量、較快的吸附速率,且吸附行為符合Langmuir等溫線模型和準二級動力學模型。其中,Pb-IIMS-MCM-41具有最優(yōu)的吸附性能及優(yōu)良的可循環(huán)能力。因此,選取Pb-IIMSMCM-41為填充材料以構建固相萃取柱,并與電感耦合等離子體質(zhì)譜(ICP-MS)聯(lián)用,對水中的痕量鉛離子進行檢測,檢出限為0.0150μg L~(-1),并在實際水樣的檢測中進行了應用,為選擇性分離和檢測水中鉛離子提供了較為有效的方法。3.巰基丙酸包覆的硒化鎘量子點(CdSe QDs)的合成及對鉛離子檢測。采用水熱法,以巰基丙酸為穩(wěn)定劑,新制備的鎘前驅體溶液和硒前驅體溶液為原料,制備了水溶性Cd Se QDs,并優(yōu)化了鎘和硒前驅體的配比與合成時間。通過了紫外光譜、熒光光譜、紅外光譜對Cd Se QDs進行了表征�？疾炝税l(fā)光體系中的p H、電位掃描速度對Cd Se ECL信號的影響。在優(yōu)化條件下測試了鉛離子對Cd Se量子點ECL信號的響應,初步建立了一種液相ECL測定鉛離子的方法,其檢出限為0.35 n M(0.072μg L~(-1))。
[Abstract]:Lead ions exist widely in the environment, because of its toxicity and in the organism can accumulate, pose a serious threat to human and organism. At present, a method for detection of lead ion has actual tend to have complicated pretreatment, high detection limit, the problem of poor selectivity. Because of this, the establishment of a reliable, high sensitive is important method for highly selective separation and detection of lead ion. The functional nanomaterials two types this paper prepared: lead ion imprinted mesoporous silicon bipyrazole functionallization and optical properties of mercaptopropionic acid package CdSe quantum dots (Cd Se QDs) is the the functionalized mesoporous silica materials used as fillers to solid phase extraction and selective separation of lead ion, and inductively coupled plasma mass spectrometry (inductively coupled plasma-atomic mass spectrometry, ICP-MS) combined with the separation and detection of lead ion in water Test. Secondly, constructed based on Cd quantum dots Se liquid phase electrochemiluminescence (electrochemiluminescence, ECL) method for detection of lead ion. The detailed work includes the following three aspects: 1. design and synthesis of lead ion imprinted mesoporous silicon material three containing nitrogendentates imprinted material modification. In 4- (two (1- hydrogen pyrazole) methyl phenol) as functional monomer, lead ion as a template, 3- carbimide propyl triethoxysilane as crosslinking agent, SBA-15 mesoporous silica materials with different morphologies were MCM-41 and FDU-12 respectively, as the solid carrier, using surface imprinting technique after template removal after Pb-IIMS-SBA-15, Pb-IIMS-MCM-41 and Pb-IIMS-FDU-12 imprinted mesoporous materials. By infrared spectroscopy, solid-state silicon spectrum and carbon spectrum proved that the functional monomer has been successfully modified on the surface of mesoporous materials; scanning electron microscope, transmission electron microscope, X ray diffraction and small angle The nitrogen adsorption desorption characterization proved that the material remained the original morphology of mesoporous silica. By energy dispersive X ray elemental analysis showed that Pb-IIMS-MCM-41 had the highest nitrogen content. In addition, three corresponding non imprinted materials are also successful preparation of.2. lead ion imprinted mesoporous silicon adsorption and its application in water samples in the analysis of lead. Imprinted material and corresponding non imprinted material adsorption capacity and selectivity were investigated. The results show that the mesoporous silicon material after imprinting of lead ions on the adsorption capacity and selectivity is increased significantly. The adsorption isotherms and adsorption kinetics experiments showed that the three materials have imprinted adsorption the larger of lead ion, the adsorption rate is relatively fast, and the adsorption behavior with the Langmuir isotherm model and the quasi two level dynamic model. Among them, Pb-IIMS-MCM-41 has the best adsorption performance and Excellent cycle ability. Therefore, selecting Pb-IIMSMCM-41 as filling material to build a solid phase extraction column, and inductively coupled plasma mass spectrometry (ICP-MS) combined with trace lead ion in water were detected, the detection limit was 0.0150 g L~ (-1), and were used in the actual sample testing, provide the effective method of.3. mercaptopropionic acid coated CdSe quantum dots for selective separation and determination of lead ion (CdSe QDs) and the synthesis of lead ion detection. By hydrothermal method with 3-mercaptopropionic acid as stabilizer, cadmium and selenium precursor solution precursor solution was prepared as raw materials, preparation the water soluble Cd Se QDs, and the optimal ratio of cadmium and selenium precursors and synthesis time. UV spectra, the fluorescence spectra of Se by Cd, QDs was characterized by infrared spectroscopy. The research of the luminescence system p H, Cd Se ECL potential scan rate on the signal. The response of lead ions to Cd Se quantum dot ECL signal was tested under optimized conditions. A method for the determination of lead ion by liquid ECL was preliminarily established. The detection limit is 0.35 n M (0.072 g L~ (-1)).

【學位授予單位】：上海師范大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：O658;TB383

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本文編號：1375233