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MO_x电极的制备与改性及电催化氧化有机废水的研究

发布时间:2019-06-17 12:51
【摘要】:本文利用静电纺丝法制备了单组份金属氧化物电极,用于电催化有机废水,对其催化活性进行筛选。对优选的单组份金属氧化物电极进行双组份混纺,制备出双金属复合电极和稀土金属铈改性的SnO2电极,电催化氧化有机废水。通过扫描电子显微镜(SEM)、X射线衍射(XRD)、线性扫描伏安法(LSV)和循环伏安法(CV)等手段对制备所得的电极材料的形貌、结构及其电化学性能进行了表征。通过紫外分光光度法(UV)、化学需氧量(COD)和总有机碳分析(TOC)对电极的催化性能进行评价。本文中以苯酚、亚甲基蓝和刚果红为模型污染物,初始浓度为200mg/L,0.25mol/L的NaN03为电解质,电流密度为30 mA/cm2,极板间的距离为2 cm,溶液初始pH为7的体系下电催化处理280 min。本研究主要分三个部分:单组份金属的筛选;Co(Fe)-SnO2复合电极的制备与电催化性能研究;Ce改性SnO2电极的制备及电催化性能的研究。得到的主要结论如下:(1)用静电纺丝法制备的单组份金属氧化物电极(SnO2、Co3O4、Fe2O3、MnOx、CuO);通过SEM、XRD和电化学表征,可以得出SnO2电极,其纤维表面连续,直径较细,且分布均匀,析氧电位高。通过紫外分光光度法(UV)、化学需氧量(COD)和总有机碳分析(TOC)对电极的催化性能进行评价;可以得出SnO2电极分别在电催化苯酚废水、亚甲基蓝废水和刚果红废水中具有较高的电催化活性。综上可以得出在单组份金属氧化物电极催化活性的筛选中SnO2电极优越。(2)对SnO2电极的制备条件和电催化条件进行优化。通过改变升温速率、煅烧温度、电流密度、环境温度和溶液的初始pH值。实验结果表明:升温速率为3 ℃/min,煅烧温度为550℃时,SnO2电极的催化效果最好,亚甲基蓝废水的脱除率、COD的去除率和TOC的去除率分别为93.2%、66.3%和75.2%。电流密度为40 mA/cm2,环境温度为40℃和溶液初始pH值为5具有最好的催化效果。(3)通过在纺丝液中掺杂不同量的C10H14CoO4(C15H21FeO6)和SnCl4·5H2O制备出Co(Fe)-SnO2复合电极;在掺杂C10H14CoO4的量与SnCl4·5H2O的质量之比为50%条件下,Co-SnO2电极的亚甲基蓝脱除率、COD去除率和TOC去除率分别为94.5%、66.4%和77.4%;在掺杂C15H21Fe06的量与SnCl4·5H20的质量之比为75%时,Fe-Sn02电极的亚甲基蓝脱除率、COD去除率和TOC去除率分别为93.9%、63.2%和74.2%。综上可以得出,Co-SnO2复合电极和Fe-Sn02复合电极的电催化活性均比单组份金属的SnO2、Co3O4和Fe2O3电极催化活性高。(4)掺杂Ce(N03)3·6H2O对SnO2电极进行改性,制备了Ce改性的Sn02电极作为阳极电催化处理亚甲基蓝废水;在掺杂硝酸铈的量与五水四氯化锡的质量比为3%条件下,Ce改性SnO2电极的电催化活性最高,亚甲基蓝废水脱除率、COD去除率和TOC去除率分别为95.2%、67.7%和79.2%。
[Abstract]:In this paper, one-component metal oxide electrode was prepared by electrospinning method, which was used to screen the catalytic activity of electrocatalytic organic wastewater. The bimetallic composite electrode and rare earth cerium modified SnO2 electrode were prepared by two-component blending of the optimized one-component metal oxide electrode to electrocatalytic oxidation of organic wastewater. The morphology, structure and electrochemical properties of the prepared electrode materials were characterized by scanning electron microscope (SEM),) X-ray diffraction (XRD), linear scanning Voltammetric method (LSV) and cyclic Voltammetric method (CV). The catalytic performance of the electrode was evaluated by UV spectrophotometry (UV), chemical oxygen demand (COD) and total organic carbon analysis (TOC). In this paper, phenol, methylene blue and Congo red were used as model pollutants, the initial concentration was 200 mg 路L, 0.25 mol 路L NaN03 was used as electrolyte, and the current density was 30 mA/cm2,. The distance between the plates was 2 cm,. The initial pH was 7. The electrocatalytic treatment of 280 min. was carried out. This study is divided into three parts: the preparation and electrocatalytic performance of; Co (Fe)-SnO2 composite electrode and the preparation and electrocatalytic performance of Ce modified SnO2 electrode. The main conclusions are as follows: (1) one-component metal oxide electrode (SnO2,Co3O4,Fe2O3,MnOx,CuO) prepared by electrospinning can be obtained by SEM,XRD and electrochemical characterization. The fiber surface of SnO2 electrode is continuous, the diameter is fine, and the distribution is uniform, and the oxygen evolution potential is high. The catalytic performance of (UV), chemical oxygen demand (COD) and total organic carbon analysis (TOC) was evaluated by UV spectrophotometry, and it was concluded that SnO2 electrode had high electrocatalytic activity in electrocatalytic phenol wastewater, methylene blue wastewater and Congo red wastewater, respectively. In summary, it can be concluded that SnO2 electrode is superior in the screening of catalytic activity of one-component metal oxide electrode. (2) the preparation and electrocatalytic conditions of SnO2 electrode are optimized. By changing the heating rate, calcination temperature, current density, ambient temperature and the initial pH value of the solution. The experimental results show that when the heating rate is 3 鈩,

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