石墨烯与血红素复合新材料的制备及其应用

发布时间：2018-05-16 11:22

本文选题：QG@PDA + 铜离子　；参考：《曲阜师范大学》2016年硕士论文

【摘要】：化学生物传感器具有设计简单、操作方便、价格低廉、灵敏度高、易于携带和检测快速等优点。本论文基于球形石墨烯(QG)和血红素(Hem),分别结合多巴胺(DA)和蛋白质,发展了石墨烯@聚多巴胺(QG@PDA)荧光材料的制备方法及其用于铜离子的荧光分析、石墨烯-血红素纳米模拟酶的制备方法及其用于环境毒物的降解、以及以血红素与牛血清白蛋白为材料制备模拟酶的方法并考察了其催化性能。(1)发展了一种基于石墨烯@聚多巴胺材料的荧光传感器并用于铜离子的分析(第二章)。以球状QG纳米材料作为支架,在微波条件下,采用过氧化氢氧化多巴胺形成的聚多巴胺膜,合成了荧光QG@PDA纳米复合材料。结果表明,QG@PDA纳米复合材料的荧光强度是PDA强度的1.5倍,而铜离子对其的猝灭程度是对PDA猝灭程度的2倍;通过对QG@PDA纳米复合材料和PDA纳米颗粒的荧光特性以及铜离子猝灭程度的对比,考察了QG@PDA纳米复合材料检测铜离子的性能,实现了对废水中铜离子的快速检测,检测范围为25 nM-50μM。此外,QG@PDA纳米材料尚可用于细胞成像,为活体中铜离子的检测提供了一个新思路。(2)基于血红素、金纳米簇、和球形石墨烯的磁性复合模拟酶的制备及其用于环境毒物的降解(第三章)。以氯化血红素为稳定剂和还原剂,一锅式反应合成了具有过氧化物酶催化活性的高稳定性血红素-金(Hem-Au)纳米复合材料,并研究了其结构和催化活性,进而将此复合材料与球形石墨烯、Fe3O4和海藻酸钠(SA)相结合,并滴入氯化钙溶液,形成(SA-Hem-Au-QG-Fe3O4)磁性复合模拟酶,并系统地研究了其催化活性。结果表明,与血红素相比,该磁性模拟酶具有更高的催化活性。此外,系统地研究了磁性模拟酶对染料的催化降解活性,发现其对亚甲基蓝和罗丹明B等有机染料具有良好的降解性能,该磁性模拟酶可采用磁铁吸取进行回收和重复利用,可望广泛地应用于环境毒物的降解。(3)通过活化氯化血红素上羧基,使之与牛血清白蛋白(BSA)中氨基酸残基交联,制备了一种血红素-牛血清白蛋白(Hem-BSA)模拟酶(第四章)。采用比色法系统地研究了该模拟酶与氯化血红素的催化活性及其反应动力学。研究表明,与氯化血红素相比,所制得的Hem-BSA模拟酶不仅获得了更高的催化性能(催化活性约是氯化血红素的4倍),而且获得了更高的反应底物亲和性;采用该模拟酶实现了对过氧化氢的检测,获得线性检测范围为0.015-2.5 mM;这种将过氧化物酶催化活性中心与蛋白质复合制备模拟酶的途径,为制备高催化活性的生物模拟酶提供了新思路,可望进一步推广于各类模拟酶的制备与催化应用领域。
[Abstract]:Chemical biosensor has the advantages of simple design, convenient operation, low price, high sensitivity, easy to carry and rapid detection. In this paper, based on spherical graphene (QG) and heme hemin (hemin), combined with dopamine (DAA) and protein respectively, the preparation method of graphene @ polydopamine QG @ PDAs and its application in the fluorescence analysis of copper ions were developed. Preparation of graphene-heme nanomimetic enzyme and its application in degradation of environmental poisons, A fluorescent sensor based on graphene @ polydopamine was developed and used for the analysis of copper ions. The fluorescent QG@PDA nanocomposites were synthesized using spherical QG nanomaterials as scaffolds and polydopamine films formed by oxidation of dopamine with hydrogen peroxide under microwave conditions. The results show that the fluorescence intensity of QG @ PDA nanocomposites is 1.5 times of that of PDA, and the quenching degree of copper ion is 2 times that of PDA. By comparing the fluorescence characteristics of QG@PDA nanocomposites and PDA nanoparticles and the quenching degree of copper ions, the properties of QG@PDA nanocomposites for copper ion detection were investigated, and the rapid detection of copper ions in wastewater was achieved. The detection range was 25 nM-50 渭 m. In addition, QG @ PDA nanomaterials can be used for cell imaging, providing a new idea for the detection of copper ions in vivo. Preparation of magnetic complex mimic enzyme and its application in the degradation of environmental toxicants (Chapter 3). Using hemin as stabilizer and reducing agent, a high stability heme-gold heme-Au-composite with peroxidase catalytic activity was synthesized by one-pot reaction, and its structure and catalytic activity were studied. Furthermore, the composite was combined with spherical graphene (Fe3O4) and sodium alginate (SA), and then dripped into calcium chloride solution to form a magnetic complex mimic enzyme, and its catalytic activity was systematically studied. The results showed that the magnetic mimic enzyme had higher catalytic activity than heme. In addition, the catalytic degradation of dyes by magnetic mimic enzyme was systematically studied. It was found that magnetic mimic enzyme had good degradation performance for organic dyes such as methylene blue and rhodamine B. the magnetic mimic enzyme could be recovered and reused by magnets. A heme-bovine serum albumin (BSA) mimic enzyme was prepared by activating the carboxyl group of hemin and crosslinking it with amino acid residues in bovine serum albumin (BSA). The catalytic activity and reaction kinetics of the mimic enzyme with hemin were systematically studied by colorimetric method. The results showed that compared with hemin, the Hem-BSA mimic enzyme not only obtained higher catalytic performance (the catalytic activity was about 4 times of hemin, but also obtained higher substrate affinity; A linear detection range of 0.015-2.5 mm was obtained by using the mimic enzyme to detect hydrogen peroxide, which is a way of synthesizing the mimic enzyme by combining the catalytic active center of peroxidase with protein. It provides a new idea for the preparation of biologic mimic enzymes with high catalytic activity and is expected to be applied to the preparation and application of various kinds of mimic enzymes.
【学位授予单位】：曲阜师范大学
【学位级别】：硕士
【学位授予年份】：2016
【分类号】：O657.3

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