单过硫酸氢钾复合盐活化技术的研究

发布时间：2018-04-14 03:31

本文选题：高级氧化技术 + 过渡金属　；参考：《河北科技大学》2017年硕士论文

【摘要】：随着人们对环保意识的提高,人们对环境改善的技术越来越关注,特别是对染料废水的处理。染料废水是经典的难消除有机废水,而偶氮染料的总量占印染废水总量的一半以上,并且它还具有染料废水的一些顽疾特点。单过硫酸氢钾复合盐(PMS)经过催化后,释放大量的硫酸自由基,可降解羟基自由基不能降解的有机污染物,将其分解为水、二氧化碳以及简单无机物。因此,研究高效活化PMS技术的方法是必要的。本文主要采用过渡金属活化PMS,通过氧化降解次甲基蓝,探讨过渡金属催化剂的催化能力。分别采用过渡金属离子(Fe~(2+)、Cu~(2+))、过渡金属氧化物(Fe_2O_3、CuO、CuFe_2O_4)、负载型过渡金属氧化物(GO-CuFe_2O_4)催化PMS氧化降解模拟次甲基蓝(MB)染料废水,得到主要结论如下:1)利用过渡金属离子(Fe~(2+)、Cu~(2+))活化PMS氧化降解MB染料废水。在Fe~(2+)/PMS体系中,可分为快速反应阶段和慢速反应阶段,而在Cu~(2+)/PMS体系中,其表观反应速率与MB呈现良好的线性关系。Fe~(2+)/PMS体系适合偏酸性情况下氧化降解MB,而Cu~(2+)/PMS体系适合在偏碱情况下氧化降解MB。此外,通过自由基抑制实验表明,Fe~(2+)/PMS、Cu~(2+)/PMS体系的主要活性自由基均为SO4-·。2)利用柠檬酸盐燃烧法制备了CuO、Fe_2O_3、CuFe_2O_4催化剂。用X射线衍射、红外光谱对制得的CuO、Fe_2O_3、CuFe_2O_4进行了表征,结果表明过度金属氧化物纳米材料的主要成分分别为CuO、Fe_2O_3及含有磁性的CuFe_2O_4。通过单因素实验对比研究了CuO/PMS、Fe_2O_3/PMS、CuFe_2O_4/PMS体系的氧化能力,结果表明,CuFe_2O_4催化活性最高。通过自由基抑制实验表明,CuO/PMS、Fe_2O_3/PMS、CuFe_2O_4/PMS体系的主要活性自由基分别为HO·、HO·、SO4-·。另外,研究表明CuFe_2O_4具有杰出的重用性。3)采用Hummers法制取氧化石墨,通过GO负载CuFe_2O_4的方法制备出GO-CuFe_2O_4。XRD与FT-IR表征结果均表明,负载型过度金属氧化物磁性纳米材料的主要成分为GO和含有磁性的CuFe_2O_4。通过单因素实验研究了GO-CuFe_2O_4/PMS体系的氧化能力。此外,与CuFe_2O_4/PMS体系对比可发现,GO-CuFe_2O_4/PMS体系的主要活性自由基同样是SO4-·,并且GO-CuFe_2O_4的催化活性优于CuFe_2O_4,而且GO-CuFe_2O_4催化剂的重用性更好。
[Abstract]:With the increasing awareness of environmental protection, people pay more and more attention to the technology of environmental improvement, especially the treatment of dye wastewater.Dyestuff wastewater is a classical organic wastewater, and the total amount of azo dyes accounts for more than half of the total printing and dyeing wastewater, and it also has some characteristics of dyestuff wastewater.After catalyzing, PMSs can release a large amount of sulfuric acid free radicals, which can degrade organic pollutants which can not be degraded by hydroxyl radicals, and decompose them into water, carbon dioxide and simple inorganic substances.Therefore, it is necessary to study the method of high efficiency activated PMS technology.In this paper, transition metal activated PMSs were used to degrade methylene blue, and the catalytic activity of transition metal catalysts was discussed.PMS was used to catalyze the oxidation and degradation of simulated methylene blue blue (MBB) dye wastewater by using transition metal ions (TME), transition metal ions (TME), transition metal oxides (TME), Fe2O3 / CuOFe2O4, supported transition metal oxides (GO-CuFe2O4), and transition metal oxides (TME) for catalytic degradation of methylene blue blue (MBB) dyestuff wastewater.The main conclusions are as follows: (1) PMS was used to oxidize and degrade MB dye wastewater.In Fe~(2 / PMS system, it can be divided into rapid reaction stage and slow reaction stage, but in Cu~(2 / PMS system,The apparent reaction rate showed a good linear relationship with MB. The system was suitable for oxidative degradation of MBs under partial acid condition, while that of Cu~(2 / PMS system was suitable for oxidative degradation of MBs under the condition of partial alkalinity.In addition, the results of free radical inhibition experiments show that the main active free radicals in the system are so _ 4-. 2) CuOO _ (Fe _ 2O _ 2O _ 3C _ S _ Fe _ 2O _ 4) catalysts have been prepared by citrate combustion method in the system of CuO / Fe2O3 / PMS / PMS / PMS / PMS / PMS / PMS / PMS / PMS / PMS / PMS system respectively.The CuO- Fe2O3 / CuFe2O4 was characterized by X-ray diffraction and infrared spectroscopy. The results show that the main components of the over metal oxide nanomaterials are CuO- Fe2O3 and CuFeSn2O4 respectively.The oxidation ability of CuO / PMS-Fe2Os 3 / PMS-CuFe2O4 / PMS system was studied by single factor experiments. The results show that CuFe2O4 has the highest catalytic activity.The results of free radical inhibition experiments show that the main active free radicals of CuO / PMS-Fe2OS / PMS3 / PMS-CuFe2O4 / PMS system are Ho / Ho / so _ 4-, respectively.In addition, the study showed that CuFe_2O_4 has excellent reusability. 3) Graphite oxide was prepared by Hummers method, and GO-CuFe_2O_4.XRD and FT-IR were prepared by GO-supported CuFe_2O_4 method.The main components of the loaded overloaded metal oxide magnetic nanomaterials are go and CuFe _ 2O _ 2 containing magnetic materials.The oxidation ability of GO-CuFe_2O_4/PMS system was studied by single factor experiment.In addition, compared with CuFe_2O_4/PMS system, it is found that the main active radical in the GO-CuFe2O4 / PMS system is also SO4-, and the catalytic activity of GO-CuFe_2O_4 is better than that of CuFe2O4, and the reusability of GO-CuFe_2O_4 catalyst is better.
【学位授予单位】：河北科技大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X791;O643.36

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