磁性過(guò)渡金屬氧化物催化類芬頓反應(yīng)降解有機(jī)染料
本文選題:鐵酸鎳 + 硫修飾改性鐵酸鈷。 參考:《西北師范大學(xué)》2015年碩士論文
【摘要】:近年來(lái),隨著工業(yè)廢水的排放量不斷增加以及淡水資源的不斷減少,越來(lái)越多的化學(xué)工作者致力于工業(yè)廢水的凈化與再生的研究。其中,以類芬頓反應(yīng)為基礎(chǔ)的高級(jí)氧化技術(shù)(AOPs)由于其高效的反應(yīng)性能以及較好的可行性受到了更多的關(guān)注。本研究以活性金屬氧化物催化H_2O_2產(chǎn)生羥基自由基進(jìn)行氧化的類芬頓反應(yīng)體系降解水溶液中的有機(jī)染料為目的,分別通過(guò)溶膠-凝膠法和共沉淀法制備了NiFe_2O_4和CoFe_2O_4兩種非均相反應(yīng)催化劑,并對(duì)后者進(jìn)行了硫元素的修飾。研究過(guò)程中分別選定了孔雀石綠(MG)和酸性橙II(AOII)兩種有機(jī)染料為降解目標(biāo)底物,通過(guò)控制變量法考察了煅燒溫度、初始pH值、參加反應(yīng)的各成分用量等一系列因素對(duì)催化效果的影響。此外,對(duì)于催化劑的穩(wěn)定性和反應(yīng)機(jī)理也進(jìn)行了較為深入的討論。通過(guò)研究得到了以下結(jié)論:(1)溶膠-凝膠法制得的NiFe_2O_4催化劑經(jīng)過(guò)XRD、BET、SEM的測(cè)試表明其尺寸較小,分散均勻,屬于納米顆粒;以其在溫度298 K、催化劑用量1.0 g·L-1、H_2O_2濃度20 mM、初始pH=7的條件下對(duì)25 mg/L的孔雀石綠水溶液進(jìn)行降解,反應(yīng)40 min后降解脫色率可達(dá)99%以上。(2)通過(guò)共沉淀法制得CoFe_2O_4顆粒并用0.5 M稀硫酸進(jìn)行修飾進(jìn)而在高溫下煅燒得到S-CoFe_2O_4催化劑。經(jīng)過(guò)XRD、BET、SEM、FT-IR、VSM表征證實(shí)了該催化劑是分散性較好并且粒度均勻的磁性納米顆粒。(3)以其在溫度298 K、催化劑用量0.1 g·L-1、H_2O_2濃度6 mM、初始pH=6的條件下對(duì)50 mg/L的酸性橙II水溶液進(jìn)行降解,反應(yīng)30 min后降解脫色率可達(dá)98%以上,同時(shí)總有機(jī)碳(TOC)的去除率也達(dá)到了40%。在后續(xù)的催化劑回收重復(fù)試驗(yàn)過(guò)程中,發(fā)現(xiàn)回收過(guò)程對(duì)兩種催化劑的性能均有一定的影響,通過(guò)XRD、BET以及EDS的表征對(duì)后者催化性能的下降進(jìn)行了較為深入的討論。
[Abstract]:In recent years, with the increasing discharge of industrial wastewater and the decreasing of fresh water resources, more and more chemical workers devote themselves to the study of purification and regeneration of industrial wastewater. Among them, advanced oxidation technology based on Fenton reaction (AOPs) has attracted more and more attention because of its high efficiency and good feasibility. The purpose of this study was to degrade organic dyes in aqueous solution by a Fenton-like reaction system catalyzed by active metal oxides to produce hydroxyl radical from H_2O_2. Two heterogeneous catalysts, NiFe_2O_4 and CoFe_2O_4, were prepared by sol-gel method and co-precipitation method, respectively, and the latter was modified by sulfur element. Two kinds of organic dyes, malachite green (MG) and acidic orange (IIAOII), were selected as the target substrate in the study. The calcination temperature and initial pH value were investigated by means of variable control method. The effect of a series of factors, such as the amount of each component involved in the reaction, on the catalytic effect. In addition, the stability and reaction mechanism of the catalyst were also discussed. The following conclusions are obtained: (1) the NiFe_2O_4 catalyst prepared by sol-gel method has been tested by XRDX BETSEM. The results show that the catalyst is small in size, uniform in dispersion and belongs to nanometer particles. The malachite green aqueous solution of 25 mg/L was degraded at 298K temperature, 1.0 g L-1 H2O2 concentration of 20mm, initial pH=7, and the amount of catalyst was 1.0 g / L ~ (-1) H _ 2O _ 2. After 40 min reaction, the decolorization rate can reach over 99%. The CoFe_2O_4 particles were prepared by coprecipitation method and modified with 0.5M dilute sulfuric acid, and then calcined at high temperature to obtain S-CoFe_2O_4 catalyst. It was confirmed by the characterization of XRDD-BETSE-SEMT-IRT-IRSM that the catalyst was a magnetic nanoparticles with good dispersion and uniform particle size. At 298K, the amount of catalyst 0.1 g / L ~ (-1) H _ 2O _ 2 was 6 mm, and the acid orange II solution of 50 mg/L was degraded under the initial pH=6 condition. The decolorization rate was over 98% after 30 min reaction, and the removal rate of total organic carbon (TOC) was 40%. In the subsequent repeated experiments of catalyst recovery, it was found that the recovery process had a certain effect on the performance of the two catalysts. The degradation of the catalytic performance of the latter was discussed through the characterization of XRD-BET and EDS.
【學(xué)位授予單位】:西北師范大學(xué)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2015
【分類號(hào)】:O643.36;X703
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