本文關(guān)鍵詞： 汞離子 電化學(xué)傳感 檢測和除去 熒光增強(qiáng)探針 環(huán)境和生物體分析　出處：《華東師范大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

【摘要】：近年來,隨著工業(yè)不斷發(fā)展,重金屬離子污染也日趨嚴(yán)重,其中,汞離子(Hg~(2+))作為一種對環(huán)境及生物體有毒的重金屬污染離子,不僅對人類的消化系統(tǒng)、神經(jīng)系統(tǒng)、肝臟以及其他器官有嚴(yán)重?fù)p傷,而且對其他物種同樣損傷嚴(yán)重。所以,美國環(huán)境保護(hù)署(EPA)和世界健康組織(WHO)規(guī)定,在飲用水中能檢測到的Hg~(2+)濃度必須小于2ppb。除此之外,汞污染也十分嚴(yán)重,為了處理汞污染,人們不僅需要開發(fā)新材料檢測更低濃度的Hg~(2+),更重要的是還能將其從溶液中快速移除。因此,發(fā)展一種高靈敏的可用于環(huán)境及生物體中Hg~(2+)的檢測并移除的新方法具有非常重要的意義。本文主要采用電化學(xué)傳感和熒光增強(qiáng)兩種分析方法,設(shè)計并開發(fā)具有高性能的Hg~(2+)探針,實(shí)現(xiàn)了對Hg~(2+)高靈敏高準(zhǔn)確度的檢測,具體內(nèi)容如下:(一)我們設(shè)計并制備了一種超靈敏比率型電化學(xué)傳感器,可準(zhǔn)確檢測和除去水中Hg~(2+),并成功實(shí)現(xiàn)了環(huán)境水樣和生物體中Hg~(2+)含量的檢測。首先,我們設(shè)計并合成了能夠與Hg~(2+)特異性結(jié)合的有機(jī)功能分子苯基硫脲(phenyl thiourea,PT),并將識別分子PT修飾到電極表面制備了性能穩(wěn)定的汞離子傳感器。該傳感器具有良好的選擇性,不受其他金屬離子和氨基酸的影響。其次,采用了電沉積金和金納米球放大信號的方法,將Hg~(2+)的測定靈敏度顯著提高了 5.3倍。與此同時,將內(nèi)參比HS-DNA-MB(MB =Methylene Blue)分子共組裝于三維納米金電極表面,構(gòu)筑了檢測Hg~(2+)的比率型電化學(xué)探針。該方法在1nM～1.3 μM范圍內(nèi)呈現(xiàn)良好線性關(guān)系,檢測限低至0.12 nM(0.024 ppb),完全可以滿足WHO和EPA的檢測需求。最后,我們將該傳感成功應(yīng)用于實(shí)際水樣和斑馬魚中Hg~(2+)的檢測。檢測結(jié)果與傳統(tǒng)電感耦合等離子體質(zhì)譜法(ICP-MS)一致,證明我們的檢測方法更簡單準(zhǔn)確,成本更低。更重要的是,該比率型電化學(xué)探針可用于痕量汞的高效率移除,移除效率高達(dá)99%。(二)我們開發(fā)了一種基于熒光增強(qiáng)原理來檢測Hg~(2+)的新型熒光探針。首先,制備了多種金屬納米材料,結(jié)果表明,不同長徑比的金納米棒與傳統(tǒng)的球形納米顆粒相比具有良好的熒光增強(qiáng)效果。然后通過靜電作用實(shí)現(xiàn)了金納米棒與能夠特異性識別Hg~(2+)的熒光染料相結(jié)合,通過多聚物層層自組裝優(yōu)化了熒光增強(qiáng)效果最佳的距離,制備了無機(jī)-有機(jī)的Hg~(2+)測定體系,實(shí)現(xiàn)了 Hg~(2+)的檢測,該方法有望用于細(xì)胞中Hg~(2+)的檢測。
[Abstract]:In recent years, with the continuous development of industry, the pollution of heavy metal ions is becoming more and more serious. Not only are there serious damage to the human digestive system, nervous system, liver and other organs, but also to other species. The Environmental Protection Agency (EPA) and the World Health Organization (WHO) require that the concentration of Hg~(2 detectable in drinking water must be less than 2 ppb. in addition, mercury pollution is very serious. In order to deal with mercury pollution, it is necessary not only to develop new materials to detect lower concentrations of Hg~(2, but also to remove it quickly from solution. It is of great significance to develop a highly sensitive method for the detection and removal of Hg~(2 in the environment and organisms. In this paper, two analytical methods, electrochemical sensing and fluorescence enhancement, are used. The Hg~(2 probe with high performance is designed and developed to detect Hg~(2 with high sensitivity and accuracy. The main contents are as follows: (1) We have designed and fabricated an ultra-sensitive ratio electrochemical sensor, which can accurately detect and remove Hg~(2 in water. And has successfully realized the environmental water sample and the organism Hg~(2 content detection. First. We have designed and synthesized phenyl thioureaPTs, an organic functional molecule that can specifically bind to Hg~(2. The recognition molecule PT was modified to the electrode surface to prepare a stable mercury ion sensor. The sensor has good selectivity and is not affected by other metal ions and amino acids. Secondly. The sensitivity of Hg~(2 was increased by 5.3 times by using electrodeposition of gold and gold nanospheres to amplify the signal. The internal reference HS-DNA-MB(MB methylene Blue molecules were co-assembled on the surface of three-dimensional gold nanocrystalline electrode. A ratio electrochemical probe for the detection of Hg~(2 was constructed, and the linear range of the method was 1. 3 渭 m. The detection limit is as low as 0. 12 nM(0.024 PbBX, which can completely meet the detection requirements of WHO and EPA. Finally. We have successfully applied the sensor to the detection of Hg~(2 in real water samples and zebrafish. The results are consistent with the conventional ICP-MS method. It is proved that our detection method is simpler, more accurate, cheaper and more important, the ratio electrochemical probe can be used for the efficient removal of trace mercury. We have developed a new fluorescent probe based on fluorescence enhancement principle to detect Hg~(2. First, we have prepared a variety of metal nanomaterials, and the results show that. The gold nanorods with different aspect ratios have good fluorescence enhancement effect compared with the traditional spherical nanoparticles. Then the gold nanorods and Hg~(2 can be specifically recognized by electrostatic action. Of fluorescent dyes. The best distance of fluorescence enhancement was optimized by layer by layer self-assembly of polymer. Inorganic-organic Hg~(2) system was prepared and the detection of Hg~(2) was realized. This method is expected to be used for the detection of Hg~(2 in cells.
【學(xué)位授予單位】：華東師范大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：O657

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本文編號：1451580