量子點分子印跡熒光傳感器的設(shè)計及其對食品污染物選擇性識別與檢測的應(yīng)用研究
發(fā)布時間:2018-06-14 01:00
本文選題:量子點 + 分子印跡; 參考:《江蘇大學》2017年碩士論文
【摘要】:食品污染問題隨著現(xiàn)代工業(yè)的發(fā)展變得日益嚴重,嚴重威脅了人類的身體健康,所以食品污染物的檢測和監(jiān)控顯得尤為重要。然而傳統(tǒng)的檢測方法預處理較為復雜、步驟繁瑣、耗時耗力,已經(jīng)漸漸不能滿足對食品污染物快速、簡便、準確檢測的需求。此外,食品種類繁多、成分復雜,需要檢測的目標物通常含量較低,需要對待測物進行分離和富集。因此,開發(fā)出選擇性好、識別快速、靈敏度高的新方法用于食品污染物的檢測已刻不容緩。分子印跡熒光傳感器結(jié)合分子印跡技術(shù)和熒光檢測技術(shù)的優(yōu)點,能夠在復雜樣品組分中準確識別并預富集痕量待檢測物,基于分子印跡熒光傳感器吸附富集待測物造成的熒光強弱變化達到目標物定量分析的效果。本文結(jié)合表面分子印跡技術(shù)和量子點熒光檢測手段,以氧化石墨烯(GO)和多孔硅為基質(zhì)材料,制備出形貌規(guī)整和能夠特異性識別食品污染物的分子印跡熒光傳感器。通過各種表征對制備的熒光傳感器的微觀結(jié)構(gòu)和表面基團進行了分析,并探討其對食品中微量污染物的識別能力和響應(yīng)速度。另外,還通過常見食品的加標回收檢測對熒光傳感器的實用性進行了考察。主要研究內(nèi)容和結(jié)果如下:(1)以Mn摻雜ZnS量子點/GO復合物為基質(zhì)材料,以丙酰胺(PAM)為偽模板,甲基丙烯酸(MAA)為功能單體,制備了一種新型的表面印跡熒光傳感器(AM-MIP)并用于檢測油炸食品中的丙烯酰胺(AM)含量。通過表征手段對這種AM-MIP的結(jié)構(gòu)和形貌進行分析,發(fā)現(xiàn)石墨烯表面形成一層均勻的印跡層。靜態(tài)吸附實驗表明AM-MIP對目標物的吸附到達平衡時間短,是一種能夠快速識別丙烯酰胺的傳感器。通過熒光檢測實驗,考察該傳感器在不同pH條件下的穩(wěn)定性、檢測范圍和熒光穩(wěn)定性,發(fā)現(xiàn)制備的熒光傳感器穩(wěn)定性高且檢測范圍廣。AM-MIP被進一步用于油炸食品中痕量AM的檢測,驗證了該熒光傳感器的實用性。(2)通過溶膠-凝膠法在ZnO量子點表面進行SiO_2包覆,以三嵌段共聚物(P123)為致孔劑,合成一種穩(wěn)定的SiO_2@ZnO多孔熒光基質(zhì)材料。以三聚氰胺(MEL)為模板,丙烯酸(AA)為功能單體,制備了能夠快速吸附MEL的分子印跡熒光傳感器(MEL-MIP)。所合成的材料隨后通過電鏡、光譜表征分析其結(jié)構(gòu)?疾炝藀H、樣品濃度、吸附時間對其識別吸附能力的影響,結(jié)果表明其是一種穩(wěn)定、響應(yīng)快速的熒光傳感器。通過熒光猝滅線性檢測確定其有較低的檢出限和寬的檢測范圍,并用于乳制品中痕量MEL的分析。(3)以SBA-15為微反應(yīng)器,糠醇(FA)為碳源前驅(qū)體,在SBA-15內(nèi)壁高溫碳化形成石墨烯,通過高溫高壓硝酸蒸氣進行氧化切割形成尺寸形貌規(guī)整的石墨烯量子點(GQDs)。以雙酚A(BPA)為模板分子,甲基丙烯酸甲脂(MMA)和L-苯丙氨酸甲酯(MAP)為功能單體,在功能化后的GO表面進行聚合,在聚合過程中引入GQDs,制備了一種新型熒光表面分子印跡傳感器(BPA-MIP)。在干擾實驗中,發(fā)現(xiàn)合成的BPA-MIP能夠選擇性識別BPA且靈敏度高。在熒光響應(yīng)實驗中,發(fā)現(xiàn)其具有較寬的檢出范圍。加標回收實驗檢測飲料樣品中BPA的含量發(fā)現(xiàn)其具有很好的回收率。(4)以檸檬酸胺和乙二胺為碳源前驅(qū)體,水熱法合成了水溶性摻氮碳量子點(NCQDs)。MAA為功能單體,4-硝基苯酚(4-NP)為模板分子,在GO表面印跡聚合物骨架中摻雜NCQDs,制備了一種對4-NP有著特異性識別吸附的分子印跡熒光傳感器(4-NP-MIP)。合成4-NP-MIP后用表征方法對其形貌和結(jié)構(gòu)進行分析,發(fā)現(xiàn)其呈現(xiàn)均勻的印跡微球包覆在二維材料表面的結(jié)構(gòu)。靜態(tài)吸附實驗研究其最佳吸附條件為pH=7.0,吸附到達平衡時間短,并對吸附參數(shù)進行分析和討論。對市場上蔬菜樣品加標分析,發(fā)現(xiàn)其具有高靈敏性和回收率。
[Abstract]:The problem of food pollution is becoming more and more serious with the development of modern industry, which seriously threatens the health of human beings. Therefore, the detection and monitoring of food contaminants is very important. However, the traditional method of preprocessing is complicated, and the steps are complicated and time-consuming. It has gradually been unable to meet the rapid, simple and accurate inspection of food contaminants. In addition, there are many kinds of food, complex ingredients, usually low content of objects to be detected and need to be separated and enriched. Therefore, a new method to detect food pollutants with good selectivity, fast recognition and high sensitivity is not slow. Molecular imprinting fluorescence sensor combined with molecular imprinting technology The advantages of the fluorescence detection technology can accurately identify and preconcentrate trace amounts in the complex sample components. The effect of fluorescence intensity changes caused by the adsorption of molecular imprinted fluorescence sensors to the quantitative analysis of the target objects is achieved. This paper combines the surface molecular trace technology and the quantum dot fluorescence detection method. Shi Moxi (GO) and porous silicon are used as matrix materials to prepare a molecularly imprinted fluorescence sensor that has a regular morphology and a specific identification of food contaminants. The microstructure and surface groups of the fluorescent sensors prepared by various characterization are analyzed, and the identification and response speed of trace contaminants in food are also discussed. The main research contents and results are as follows: (1) a new type of surface imprinted fluorescence sensor (AM-M) was prepared with Mn doped ZnS quantum dot /GO complex as matrix material, PAM as pseudo template and methacrylic acid (MAA) as power monomer. IP) was used to detect the content of acrylamide (AM) in fried foods. The structure and morphology of the AM-MIP were analyzed by means of characterization. A homogeneous layer of imprinting layer was found on the surface of graphene. The static adsorption experiment showed that the adsorption of AM-MIP on the target reached a short equilibrium time. It was a kind of fast sensor to identify the acrylamide. The stability, detection range and fluorescence stability of the sensor under different pH conditions were investigated by fluorescence detection experiments. It was found that the stability of the fluorescence sensor was high and the detection range was wide.AM-MIP was further used in the detection of trace AM in fried food. The practicability of the fluorescent sensor was verified. (2) through the sol-gel method in ZnO The quantum dot surface is coated with SiO_2, and a stable SiO_2@ZnO porous fluorescent matrix material is synthesized with three block copolymer (P123) as a pore agent. The molecular imprinting fluorescein sensor (MEL-MIP), which can quickly adsorb MEL, is prepared with melamine (MEL) as a template and acrylic acid (AA) as a functional monomer. The synthesized materials are followed by electron microscopy and light. The effect of pH, sample concentration and adsorption time on the identification of adsorption capacity was investigated. The results showed that it was a stable, fast response fluorescence sensor. By fluorescence quenching linear detection, it has a low detection limit and wide detection range, and is used for the analysis of trace MEL in dairy products. (3) SBA-15 is a micro scale. The reactor, furfuryl alcohol (FA) as a precursor of carbon source, carbonized a graphene at high temperature on the inner wall of SBA-15 and formed a structured graphene quantum dot (GQDs) by oxidation of high temperature and high pressure nitric vapor to form a structured graphene point (GQDs). With bisphenol A (BPA) as a template molecule, MMA and L- phenylalanine methyl ester (MAP) as functional monomers, after functionalization. A new fluorescent surface molecular imprinting sensor (BPA-MIP) was prepared by introducing GQDs into the GO surface. In the interference experiment, it was found that the synthesized BPA-MIP was able to identify BPA with high sensitivity. In the fluorescence response experiment, it was found that it had a wide detection range. The content of BPA was found to have good recovery. (4) using citric acid amine and ethylenediamine as the precursor of carbon source, water soluble nitrogen doped carbon quantum dots (NCQDs).MAA as functional monomers, 4- nitrophenol (4-NP) as template molecule, and NCQDs in the matrix of GO surface imprinted polymer were doped with NCQDs. A kind of specific identification adsorption on 4-NP was prepared. Molecular imprinting fluorescence sensor (4-NP-MIP). After synthesis of 4-NP-MIP, its morphology and structure were analyzed. It was found that the structure of the microspheres was coated on the surface of the two-dimensional material. The best adsorption condition was pH=7.0, the adsorption equilibrium time was short, and the adsorption parameters were analyzed and discussed. The analysis of vegetable samples in market shows that it has high sensitivity and recovery rate.
【學位授予單位】:江蘇大學
【學位級別】:碩士
【學位授予年份】:2017
【分類號】:TS207.5;O657.3
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