钌纳米粒子催化加氢性质尺寸效应研究及其分析检测应用

发布时间：2018-03-23 10:43

本文选题：钌纳米粒子　切入点：可控合成　出处：《江南大学》2017年硕士论文

【摘要】：钌作为贵金属元素,由于其空轨道多,易配位,电子多,易成键等优势使其成为理想的催化剂。众所周知,贵金属纳米的尺寸是影响其催化活性的重要因素,但是关于钌纳米粒子(Ru NPs)催化领域的尺寸效应却鲜有研究,主要原因是不同尺寸的Ru NPs难以合成,关于不同尺寸Ru NPs的催化性能研究也寥寥无几,本文以Ru NPs为研究对象,围绕其催化加氢性质尺寸效应研究及其分析检测应用展开系统研究。具体内容包括:1.通过调节pH和温度合成不同粒径Ru NPs,深入理解钌纳米粒子在形成过程中晶体成核和生长的机理,探究钌纳米粒子可控合成的规律,考察影响纳米粒子可控合成的因素。并通过一系列表征手段,对不同粒径Ru NPs的性质有了一定的了解。2.利用Ru NPs优异的催化加氢性能催化还原硝基化合物,选用了对硝基苯酚(pNP)作为芳香族硝基化合物的代表,通过高效液相色谱技术(HPLC),研究还原产物以及反应转化率;通过紫外可见分光光度计(UV-Vis)监控催化反应并计算反应速率,与其它贵金属纳米粒子催化速率比较,考察了Ru NPs的催化加氢活性;同时研究不同尺寸的Ru NPs对催化活性的影响,并深入理解现象,提出尺寸影响催化活性的机理。最后经过催化剂的循环使用测试,证明Ru NPs能够重复使用。3.利用Ru NPs优异的催化加氢性质催化降解偶氮染料,并研究其催化机理。选用偶氮染料通过UV-Vis监控染料降解脱色过程,发现加入Ru NPs催化速率比不加催化剂速率快上几十倍甚至几百倍。4.经研究发现硫化氢(H2S)可诱导Ru NPs中毒,降低Ru NPs的催化活性。将此性质与Ru NPs催化降解偶氮染料结合,建立了一种快速、高灵敏比色检测硫化氢的方法。经过参数优化,检测限可达到0.6 nmol/L。同时经过干扰性实验测试,该检测方法表现出高选择性,并能应用于实际样品的检测。同样基于Ru NPs检测H2S的原理,该检测方法还能检测生物样品中带巯基的氨基酸,如:半胱氨酸和谷胱甘肽。因此,该检测方法能够应用于环境样品和生物样品中H2S的检测。
[Abstract]:Ruthenium, as a precious metal element, is an ideal catalyst because of its many empty orbits, easy coordination, many electrons and easy bonding. It is well known that the size of noble metal nanoparticles is an important factor affecting its catalytic activity. However, there are few studies on the size effect of Ru NPs in the field of Ru NPs. The main reason is that it is difficult to synthesize Ru NPs with different sizes, and the catalytic performance of Ru NPs with different sizes is very little. In this paper, Ru NPs is taken as the research object. A systematic study was carried out on the size effect of catalytic hydrogenation properties and its analytical application. The specific contents include: 1. Synthesis of Ru NPs with different particle sizes by adjusting pH and temperature, and in-depth understanding of Ru NPs in the formation process of ruthenium nanoparticles. The mechanism of nucleation and growth, To explore the law of controllable synthesis of ruthenium nanoparticles, to investigate the factors that affect the controllable synthesis of ruthenium nanoparticles, and through a series of characterization methods, The properties of Ru NPs with different diameters were well understood. 2. The excellent catalytic hydrogenation performance of Ru NPs was used to catalyze the reduction of nitro compounds, and p-nitrophenol was chosen as the representative of aromatic nitro compounds. High performance liquid chromatography (HPLC) was used to study the reduction products and the conversion rate of the reaction. The catalytic reaction was monitored by UV-Vis-UV spectrophotometer and the reaction rate was calculated and compared with the catalytic rate of other noble metal nanoparticles. The catalytic hydrogenation activity of Ru NPs was investigated, and the effect of Ru NPs of different sizes on the catalytic activity was studied. It is proved that Ru NPs can be reused. 3. The excellent catalytic hydrogenation property of Ru NPs is used to catalyze the degradation of azo dyes and its catalytic mechanism is studied. Azo dyes are selected to monitor the degradation and decolorization process of azo dyes by UV-Vis. It was found that the catalytic rate of Ru NPs was several times or even several hundred times faster than that of no catalyst. It was found that hydrogen sulfide (H _ 2S) could induce Ru NPs poisoning and decrease the catalytic activity of Ru NPs. This property was combined with Ru NPs to catalyze the degradation of azo dyes. A rapid and highly sensitive colorimetric method for the detection of hydrogen sulfide has been developed. The detection limit can reach 0.6 nmol / L by parameter optimization. Also based on the principle of Ru NPs detection of H2S, the method can also detect amino acids with sulfhydryl group in biological samples, such as cysteine and glutathione. The method can be applied to the detection of H _ 2S in environmental and biological samples.
【学位授予单位】：江南大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O643.36

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