發(fā)布時(shí)間：2018-10-11 09:27

【摘要】：傳統(tǒng)的均相光助Fenton反應(yīng)存在pH值適用范圍狹窄,對(duì)可見(jiàn)光的利用率低以及反應(yīng)后鐵離子難以與反應(yīng)介質(zhì)分離等缺陷。為克服均相光助Fenton反應(yīng)存在的問(wèn)題,本文制備了水滑石負(fù)載四磺酸鐵酞菁光助Fenton催化劑(FePcS-LDH),并通過(guò)將其應(yīng)用于亞甲基藍(lán)(MB)的降解反應(yīng)來(lái)測(cè)試其催化活性。此外,通過(guò)以BBD設(shè)計(jì)為基礎(chǔ)的響應(yīng)曲面分析得出Fe PcS-LDH異相光助Fenton催化降解MB的最佳實(shí)驗(yàn)條件。所得結(jié)果如下:采用傅里葉紅外光譜分析(FTIR)、X射線衍射分析(XRD)、電子掃描電鏡(SEM)、氮?dú)馕?脫附曲線以及紫外-可見(jiàn)漫反射圖譜分析(DRS)等技術(shù)對(duì)FePcS-LDH催化劑進(jìn)行表征。FTIR和XRD的表征結(jié)果表明鎂鋁水滑石(MgAl-LDH)成功負(fù)載四磺酸鐵酞菁(Fe PcS);DRS的表征結(jié)果表明FePcS-LDH催化劑對(duì)可見(jiàn)光有較強(qiáng)的吸收;氮?dú)馕?脫附曲線表明負(fù)載了Fe PcS后,水滑石的比表面積和孔體積顯著增大。在可見(jiàn)光輻射下,反應(yīng)體系pH中性范圍內(nèi),FePcS-LDH異相光助Fenton催化劑對(duì)MB的降解呈現(xiàn)出高效的催化能力。通過(guò)響應(yīng)曲面分析得出反應(yīng)的最佳條件為初始染料濃度為10.00 mg/L,雙氧水濃度為10.30 m M,可見(jiàn)光輻射強(qiáng)度為463.50 W;在最佳實(shí)驗(yàn)條件下的脫色率和礦化率分別為99.88%和76.50%。此外,在循環(huán)3次后,FePcS-LDH催化劑對(duì)MB的降解依然保持高效的催化能力,說(shuō)明其穩(wěn)定性良好。通過(guò)對(duì)活性物種的抑制實(shí)驗(yàn),考察了異相光助Fenton體系催化降解MB過(guò)程中所涉及的主要活性物種,并推斷了該活性物種的產(chǎn)生路徑,為闡明異相光助Fenton體系作用機(jī)理提供了有力的依據(jù)。
[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.
【學(xué)位授予單位】：湘潭大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類(lèi)號(hào)】：X788

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本文編號(hào)：2263691