荧光碳纳米材料的制备及其在传感器中的应用

发布时间：2018-03-18 02:32

本文选题：碳点　切入点：比率荧光　出处：《中国科学技术大学》2017年博士论文　论文类型：学位论文

【摘要】：碳纳米材料,比如纳米金刚石、富勒烯、碳纳米管、石墨烯、荧光碳纳米材料或碳点具有特殊的性质,它们在技术上具有宽范围的应用前景。特别是碳点,与其他的荧光材料相比具有很多的优点:高的光学稳定性、发射颜色可调等。碳点是一个很好的荧光探针,已经被广泛地应用于化学传感和生物成像领域。最近几年来,碳点已经成为了研究领域的热点之一。本文以不同的方法合成了颜色不同的荧光碳点,并且以重金属离子作为分析检测的目标,充分利用了碳点的表面官能团的性质,分别构建了以碳点为基础的传感方法。初步构建了对重金属离子能够实时、快速、高灵敏性检测重金属离子并且可以用裸眼观察到可视化的检测方法。另外,利用高能近红外激光器作为一种新的工具用产生发白光的二氧化硅纳米粒子,在设备和照明上具有很好的应用前景。本论文主要的研究内容如下:1.传统的pH试纸已经广泛用来定量、半定量检测物质的酸碱度。然而,发展一种便携式并且便宜的方法来用于宽范围检测分析物,这种方法可以使我们从仪器分析中解脱出来,但是一直未取得成功。我们构建了一种新型的双色碳点基础的比率荧光试纸依赖于剂量敏感的颜色变化来半定量检测铜离子。这种试纸的创新是基于两个有趣的发现:一方面:我们合成的红色碳点表面残留的对苯二胺配体可以有效得结合铜离子,从而产生了一个强的可见吸收峰,这个吸收峰可以和蓝色碳点的发射峰能够很好得重叠,另一方面:铜离子可以同时与红色碳点和蓝色碳点的表面的配体形成双配位,使得小的蓝色碳点吸附在大的红色碳点的表面。上述的两种机制产生了特定的光谱能量转移,从而猝灭了蓝色碳点的光,而红色碳点的荧光作为内标并保持不变,铜离子的检测线8.82 nM。比率荧光试纸是蓝色碳点和红色碳点(荧光强度7:1)的混合作为墨水,并且把墨水打印在滤纸上。当滴加铜离子上去后,蓝的试纸产生连续的宽范围的颜色变化,从蓝色变成橙红色,试纸的剂量分辨能力低至25 nM。2.制备的比率荧光探针用于选择性的检测汞离子,同时,探针是由发蓝光的硅纳米晶和发红光的碳点混合制备而成的。硅纳米晶作为接受信号,而红色碳点作为内标。通过加入汞离子,硅纳米晶的蓝色荧光被淬灭,而红色碳点的红色荧光保持不变。探针显示出了高的选择性和灵敏性用于可视化的检测汞离子,其检测限是7.63 nM。比率荧光试纸是把红色碳点和蓝色硅纳米晶(荧光强度1:7)的混合液作为墨水,并且把这种墨水打印在滤纸上,制成比率荧光试纸。这种比率荧光试纸显示出了实时、灵敏、快速检测汞离子的优点。3.白光材料可以应用在设备和照明上,这种材料可以通过发光效率高并且稳定的稀土得到。但是由于稀土资源的稀缺、昂贵和其带来的严重的环境问题是以稀土为基础的材料不可以逾越的障碍。由强激光诱导产生的瞬间高温和高压使得二氧化硅纳米粒子内部的部分的二氧化硅被还原和碳链的裂解,从而使得二氧化硅矩阵中的硅和碳快速地结晶,从而形成了硅点和金刚石状的碳点。非常重要的是,产生的二氧化硅纳米粒子包含了不同粒径的硅点和碳点,从而在紫外灯的照射下展示出了宽范围的荧光光谱来形成了白光。另外,发光二极管(LED)设备是由制得的发白光的二氧化硅纳米粒子作为发光源制备而成的,并且发射出的暖白光,它的国际照明委员会(CIE)参数为(0.34,0.32)。我们报道的这种方法是通过简单、便宜和环境友好的方式打开了探索白光照明材料的一扇窗。
[Abstract]:Carbon nano materials, such as nano diamond, fullerenes, carbon nanotubes, graphene, special properties of carbon nano materials with fluorescent or carbon, which has a wide application prospect in technology. Especially carbon, has many advantages compared with other fluorescent material: high optical stability, adjustable color emission. Carbon is a good fluorescent probe has been widely used in chemical and biological sensing imaging field. In recent years, carbon has become one of the hot research field. In this paper, different methods to synthesis of fluorescent carbon dots of different colors, and with heavy metal ions as detection the target, make full use of the properties of surface functional groups of carbon dots, were constructed using carbon based point sensing method. The initial construction of the heavy metal ions can be real-time, rapid, high sensitivity and the detection of heavy metal ions And can use the naked eye observation to visible detection method. In addition, as a new tool for producing white silica nanoparticles by using high-energy near-infrared laser, has good application foreground in equipment and lighting. The main research contents of this thesis are as follows: 1. the traditional pH test has been widely used for quantitative, semi quantitative detection of substance pH. However, the development of a portable and inexpensive method for a wide range of analyte detection, this method can make us free from the instrument analysis, but has not been successful. Strip ratio fluorescence we constructed a novel carbon based double color depends on the color sensitive dose the change detection of copper ions. The innovation of this paper to semi quantitative two interesting findings based on: on the one hand: we synthesized the carbon residue red surface of two benzene amine ligand Can effectively combine copper ions, resulting in a strong visible absorption peak and emission peak of the absorption peak and blue point carbon can be a very good overlap, on the other hand, the ligand surface at the same time with red and blue carbon carbon dots to form double complexing copper ions can make the surface of the blue. Carbon adsorption in little red carbon big. The two mechanisms have specific spectral energy transfer and quenching blue carbon point light, and red fluorescent carbon dots as the internal standard and remain unchanged, the 8.82 nM. line detection of copper ion ratio fluorescent strip is blue and red point carbon carbon dots (fluorescence intensity 7:1) mixed as ink, and the ink printed on the filter paper. When adding copper ions to go after the color change of blue paper produce a wide range of continuous, from blue to orange red, the resolution of low dose test to 25 nM.2. preparation The ratio of fluorescence probe for the detection of mercury ion selective probe at the same time, is a mixture of silicon nanocrystals emit blue light and red emitting carbon prepared from silicon nanocrystals. As a signal, while the red point carbon as the internal standard. By the addition of mercury ion, silicon nano crystal blue fluorescence was quenched out, while the red fluorescent red point carbon remains unchanged. The probe showed high selectivity and sensitivity for the detection of mercury ion visualization, the detection limit is 7.63 nM. ratio fluorescence test paper is the red and blue carbon silicon nanocrystals (fluorescence intensity 1:7) mixture as the ink, and the printing ink in the paper, the paper made the ratiometric fluorescence ratio. Test shows a real-time, sensitive, the advantages of.3. white material rapid detection of mercury ions can be used in equipment and lighting, this kind of material can be with high luminous efficiency and stability The rare earth rare earth. But because of the scarcity of resources, expensive and it brings serious environmental problems in rare earth based materials can not be an insurmountable obstacle. Produced by laser induced transient high temperature and high pressure makes the two silicon oxide nanoparticles inside the part is reduced and the carbon chain cleavage, which makes silicon in the matrix and carbon silica fast crystallization, thus forming a silicon and diamond like carbon. It is very important that the silica nanoparticles produced by different particle size of silicon containing point and carbon, which under the irradiation of UV lamp showing a wide range of fluorescence spectrum to form white light. In addition, the light emitting diode (LED) device is prepared by the white light as the light source of the silica nanoparticles was prepared, and the warm white light emitting, the International Commission on illumination (CIE) parameters For (0.34,0.32). The method we report is a window to explore white light materials in a simple, cheap and environmentally friendly way.

【学位授予单位】：中国科学技术大学
【学位级别】：博士
【学位授予年份】：2017
【分类号】：TQ422;TB383.1;TP212

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