镁铝水滑石负载四磺酸酞菁铁可见光—芬顿催化降解亚甲基蓝的研究
发布时间：2018-10-11 09:27
【摘要】：传统的均相光助Fenton反应存在pH值适用范围狭窄,对可见光的利用率低以及反应后铁离子难以与反应介质分离等缺陷。为克服均相光助Fenton反应存在的问题,本文制备了水滑石负载四磺酸铁酞菁光助Fenton催化剂(FePcS-LDH),并通过将其应用于亚甲基蓝(MB)的降解反应来测试其催化活性。此外,通过以BBD设计为基础的响应曲面分析得出Fe PcS-LDH异相光助Fenton催化降解MB的最佳实验条件。所得结果如下:采用傅里叶红外光谱分析(FTIR)、X射线衍射分析(XRD)、电子扫描电镜(SEM)、氮气吸附-脱附曲线以及紫外-可见漫反射图谱分析(DRS)等技术对FePcS-LDH催化剂进行表征。FTIR和XRD的表征结果表明镁铝水滑石(MgAl-LDH)成功负载四磺酸铁酞菁(Fe PcS);DRS的表征结果表明FePcS-LDH催化剂对可见光有较强的吸收;氮气吸附-脱附曲线表明负载了Fe PcS后,水滑石的比表面积和孔体积显著增大。在可见光辐射下,反应体系pH中性范围内,FePcS-LDH异相光助Fenton催化剂对MB的降解呈现出高效的催化能力。通过响应曲面分析得出反应的最佳条件为初始染料浓度为10.00 mg/L,双氧水浓度为10.30 m M,可见光辐射强度为463.50 W;在最佳实验条件下的脱色率和矿化率分别为99.88%和76.50%。此外,在循环3次后,FePcS-LDH催化剂对MB的降解依然保持高效的催化能力,说明其稳定性良好。通过对活性物种的抑制实验,考察了异相光助Fenton体系催化降解MB过程中所涉及的主要活性物种,并推断了该活性物种的产生路径,为阐明异相光助Fenton体系作用机理提供了有力的依据。
[Abstract]:The traditional homogeneous light-assisted Fenton reaction has some defects, such as narrow range of pH value, low utilization of visible light and the difficulty of separating iron ions from the reaction medium after the reaction. In order to overcome the problem of homogeneous photo-assisted Fenton reaction, a hydrotalcite supported Fe phthalocyanine tesilate photo-assisted Fenton catalyst (FePcS-LDH) was prepared, and its catalytic activity was tested by applying it to the degradation of methylene blue (MB). In addition, based on the response surface analysis based on BBD design, the optimal experimental conditions for the catalytic degradation of MB by Fe PcS-LDH heterogeneous photo-assisted Fenton were obtained. The results obtained are as follows: Fourier transform infrared spectroscopy (FTIR) analysis of (FTIR), X ray diffraction analysis of (XRD), electron scanning electron microscopy (SEM) (SEM), nitrogen adsorption and desorption curve and UV-Vis diffuse reflectance spectrum analysis (DRS) were used to characterize the FePcS-LDH catalyst. FTIR was used to characterize the FePcS-LDH catalyst. The results of XRD and Mg-Al hydrotalcite (MgAl-LDH) showed that the FePcS-LDH catalyst had strong absorption of visible light. The nitrogen adsorption-desorption curve showed that the specific surface area and pore volume of hydrotalcite increased significantly when Fe PcS was loaded. Under visible light radiation, FePcS-LDH heterogeneous photo-assisted Fenton catalyst exhibited high catalytic activity for MB degradation in the neutral range of pH. The optimum conditions for the reaction are as follows: the initial dye concentration is 10.30 mg/L, hydrogen peroxide concentration, the visible light radiation intensity is 463.50 W, and the decolorization rate and mineralization rate are 99.88% and 76.50% respectively under the optimum experimental conditions. In addition, after three cycles, the FePcS-LDH catalyst still maintained a high catalytic capacity for MB degradation, indicating that the stability of the catalyst was good. The main active species involved in the catalytic degradation of MB in heterogeneous photo-assisted Fenton system were investigated through the inhibition experiments on the active species, and the production path of the active species was inferred. It provides a powerful basis for elucidating the mechanism of heterogeneous photo-assisted Fenton system.
【学位授予单位】：湘潭大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X788
本文编号：2263691
[Abstract]:The traditional homogeneous light-assisted Fenton reaction has some defects, such as narrow range of pH value, low utilization of visible light and the difficulty of separating iron ions from the reaction medium after the reaction. In order to overcome the problem of homogeneous photo-assisted Fenton reaction, a hydrotalcite supported Fe phthalocyanine tesilate photo-assisted Fenton catalyst (FePcS-LDH) was prepared, and its catalytic activity was tested by applying it to the degradation of methylene blue (MB). In addition, based on the response surface analysis based on BBD design, the optimal experimental conditions for the catalytic degradation of MB by Fe PcS-LDH heterogeneous photo-assisted Fenton were obtained. The results obtained are as follows: Fourier transform infrared spectroscopy (FTIR) analysis of (FTIR), X ray diffraction analysis of (XRD), electron scanning electron microscopy (SEM) (SEM), nitrogen adsorption and desorption curve and UV-Vis diffuse reflectance spectrum analysis (DRS) were used to characterize the FePcS-LDH catalyst. FTIR was used to characterize the FePcS-LDH catalyst. The results of XRD and Mg-Al hydrotalcite (MgAl-LDH) showed that the FePcS-LDH catalyst had strong absorption of visible light. The nitrogen adsorption-desorption curve showed that the specific surface area and pore volume of hydrotalcite increased significantly when Fe PcS was loaded. Under visible light radiation, FePcS-LDH heterogeneous photo-assisted Fenton catalyst exhibited high catalytic activity for MB degradation in the neutral range of pH. The optimum conditions for the reaction are as follows: the initial dye concentration is 10.30 mg/L, hydrogen peroxide concentration, the visible light radiation intensity is 463.50 W, and the decolorization rate and mineralization rate are 99.88% and 76.50% respectively under the optimum experimental conditions. In addition, after three cycles, the FePcS-LDH catalyst still maintained a high catalytic capacity for MB degradation, indicating that the stability of the catalyst was good. The main active species involved in the catalytic degradation of MB in heterogeneous photo-assisted Fenton system were investigated through the inhibition experiments on the active species, and the production path of the active species was inferred. It provides a powerful basis for elucidating the mechanism of heterogeneous photo-assisted Fenton system.
【学位授予单位】：湘潭大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X788
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