【摘要】：全氟辛烷磺酸(Perfluoroocatane Sulfonate,PFOS)和全氟辛酸(Perfluoroocatanoic Acid,PFOA)是兩種具有代表性的全氟化合物(Perfluorinated Compounds,PFCs)。具有持久性,生物積累性,長(zhǎng)距離遷移性和致癌性。因此對(duì)環(huán)境中PFOS和PFOA的檢測(cè)具有十分重要的意義。本文基于共振光散射法和熒光碳量子點(diǎn)的分析技術(shù)等光學(xué)方法設(shè)計(jì)了用于檢測(cè)PFOS和PFOA的光學(xué)傳感器,探討了其反應(yīng)機(jī)理,并將其應(yīng)用于實(shí)際水樣中PFOS和PFOA含量的分析測(cè)定。主要包括以下幾個(gè)方面:(1)建立了一種用維多利亞藍(lán)B(Victoria blue B,VBB)簡(jiǎn)便,高靈敏、選擇性檢測(cè)PFOS的共振光散射(Resonance Light Scattering,RLS)分析方法。在pH 6.0的KH2PO4-NaOH緩沖體系下,PFOS通過(guò)靜電作用與質(zhì)子化的VBB結(jié)合生成離子締合物,在277 nm處的散射信號(hào)有明顯的增強(qiáng),增強(qiáng)的散射值(?IRLS)與PFOS在一定濃度范圍內(nèi)有良好的線性關(guān)系,其線性方程為?IRLS=72.28+336.53c(R2=0.9964),線性范圍為0.05-4.0μM,檢測(cè)限為5.0 nM。優(yōu)化了實(shí)驗(yàn)條件,表征了紫外/可見(jiàn)吸收光譜、掃描電鏡顯微成像(SEM),并探討了作用機(jī)理。在相同實(shí)驗(yàn)條件下,考察了PFOA及其他幾種PFCs與VBB的相互作用,未見(jiàn)散射信號(hào)變化,因此,本法可實(shí)現(xiàn)對(duì)PFOS的選擇性檢測(cè)。該方法成功應(yīng)用于檢測(cè)環(huán)境水樣中的PFOS,樣品加標(biāo)回收率在91.8%-100.6%,相對(duì)標(biāo)準(zhǔn)偏差RSD≤1.74%。(2)通過(guò)水熱法快速合成了一種具有高熒光量子產(chǎn)率且?guī)С壬珶晒獾男滦吞剂孔狱c(diǎn)(CQDs),并用其檢測(cè)復(fù)雜水樣及生物體中的PFOS以及PFOA。我們以4-(二乙基氨基)水楊醛和磷酸作為反應(yīng)原料,在200 oC下,于聚四氟乙烯內(nèi)襯不銹鋼高壓釜內(nèi)一起加熱1 h合成了上述碳量子點(diǎn)(CQDs)。強(qiáng)酸及高溫的協(xié)同作用加速了水熱反應(yīng)的速率。所得的橙色碳量子點(diǎn)的熒光量子產(chǎn)率為47.1%。我們發(fā)現(xiàn)PFOS和PFOA(PFOS/PFOA)可以通過(guò)電子轉(zhuǎn)移(ET)對(duì)制備的CQDs具有強(qiáng)烈的猝滅效應(yīng)。隨著PFOS/PFOA濃度的增加,在596 nm處的碳量子點(diǎn)熒光強(qiáng)度逐漸降低,且PFOS/PFOA濃度范圍分別為0.05-1.0μM,0.1-1.5μM。此外,由于所制備的CQDs具有較高的化學(xué)穩(wěn)定性和穩(wěn)定的光致發(fā)光能力,CQDs可用于復(fù)雜水樣甚至生物體內(nèi)的PFOS/PFOA檢測(cè)。由于該方法檢測(cè)PFOS/PFOA十分簡(jiǎn)便,因此在生物分析中具有很大的應(yīng)用前景。
[Abstract]:Perfluorooctane sulfonic acid (Perfluoroocatane Sulfonate,PFOS) and perfluorooctanoic acid (Perfluoroocatanoic Acid,PFOA) are two representative perfluorooctane compounds (Perfluorinated Compounds,PFCs). Persistent, bioaccumulative, long-distance migration and carcinogenicity. Therefore, it is very important to detect PFOS and PFOA in the environment. In this paper, an optical sensor for detecting PFOS and PFOA is designed based on the resonance light scattering method and the analytical technique of fluorescence carbon quantum dots. The reaction mechanism is discussed and applied to the analysis and determination of PFOS and PFOA contents in practical water samples. The main contents are as follows: (1) A simple, highly sensitive and selective method for the determination of PFOS by resonance light scattering (Resonance Light Scattering,RLS (RLS-(Resonance Light Scattering,RLS) was developed by using Victoria Blue B (Victoria blue B (VBB). In the KH2PO4-NaOH buffer system of pH 6.0.The ion association complex was formed by electrostatic interaction between PFOS and protonated VBB, and the scattering signal at 277 nm was obviously enhanced. The enhanced scattering value (? IRLS) has a good linear relationship with PFOS in a certain concentration range. The linear equation is? IRLS=72.28 336.53c (R2 = 0.9964), the linear range is 0.05-4.0 渭 M, and the detection limit is 5.0 nM.. The experimental conditions were optimized, UV / vis absorption spectra were characterized, scanning electron microscopy (SEM) was used to image (SEM), and the mechanism of action was discussed. Under the same experimental conditions, the interaction of PFOA and other PFCs with VBB has not been observed. Therefore, the selective detection of PFOS can be realized by this method. The method was successfully applied to the determination of PFOS, samples in environmental water samples. The recovery rate was 91.8% and 100.6%, respectively. Relative standard deviation (RSD) was 1.74%. (2) A novel carbon quantum dot (CQDs), with high fluorescence quantum yield and orange fluorescence was synthesized by hydrothermal method and used to detect PFOS and PFOA. in complex water samples and organisms. The carbon quantum dots (CQDs).) were synthesized from 4-(diethylamino) salicylaldehyde and phosphoric acid at 200 oC in a stainless steel autoclave lined with PTFE for 1 h. The synergistic action of strong acid and high temperature accelerated the rate of hydrothermal reaction. The fluorescence quantum yield of orange carbon quantum dots is 47.1%. We found that PFOS and PFOA (PFOS/PFOA) have a strong quenching effect on the prepared CQDs by electron transfer (ET). With the increase of PFOS/PFOA concentration, the fluorescence intensity of carbon quantum dots decreased gradually at 596 nm, and the concentration range of PFOS/PFOA was 0.05-1.0 渭 M and 0.1-1.5 渭 M, respectively. In addition, due to the high chemical stability and stable photoluminescence ability of the prepared CQDs, CQDs can be used for the detection of PFOS/PFOA in complex water samples and even in organisms. Because this method is very simple to detect PFOS/PFOA, it has great application prospect in biological analysis.
【學(xué)位授予單位】：西南大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類(lèi)號(hào)】：O657.3;X832

【參考文獻(xiàn)】

相關(guān)期刊論文 前10條

1 侯超峰;高國(guó)賢;徐驥;;納米材料制備及物性測(cè)量的虛擬過(guò)程工程初探[J];計(jì)算機(jī)與應(yīng)用化學(xué);2016年09期

2 儲(chǔ)誠(chéng)燦;蘇朝暉;;聚合物負(fù)載納米材料及其在催化領(lǐng)域的應(yīng)用[J];應(yīng)用化學(xué);2016年04期

3 伊魁宇;鄒寧;韓闖;王猛;;納米材料傳感器檢測(cè)硝基爆炸物的研究[J];應(yīng)用化工;2015年04期

4 鄭莉;朱進(jìn);吳飛;叢妍斌;譚克俊;;利用納米金局域表面等離子體共振散射方法檢測(cè)痕量汞(Ⅱ)[J];光譜學(xué)與光譜分析;2014年06期

5 鄧小燕;李佳渝;譚克俊;;基于碳量子點(diǎn)熒光分光光度法檢測(cè)葉酸[J];分析化學(xué);2014年04期

6 楊莉莉;金芬;李敏潔;牛云景;王靜;邵華;金茂俊;;食品和食品包裝材料中全氟化合物(PFCs)的研究進(jìn)展[J];食品工業(yè)科技;2014年08期

7 李華春;覃明麗;譚克俊;;硅鎢酸與鹽酸巴馬汀相互作用光譜研究及其分析應(yīng)用[J];化學(xué)學(xué)報(bào);2012年06期

8 陳劍君;方凱;胡鳴韻;;PFOA和PFOS檢測(cè)方法研究進(jìn)展[J];化工生產(chǎn)與技術(shù);2011年03期

9 南海軍;劉忠芳;劉紹璞;郭麗冰;問(wèn)國(guó)強(qiáng);;鉛(Ⅱ)-碘化物-溴化十四烷基吡啶三元絡(luò)合體系的共振瑞利散射光譜及其分析應(yīng)用研究[J];光譜實(shí)驗(yàn)室;2008年02期

10 賀薇;李原芳;譚克俊;黃承志;;金納米棒與肝素相互作用的表征及肝素的等離子共振光散射分析法[J];科學(xué)通報(bào);2007年24期

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