本文關(guān)鍵詞：iCWPO與光催化工藝處理染料廢水及其協(xié)同作用的實(shí)驗(yàn)研究　出處：《陜西師范大學(xué)》2015年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 感應(yīng)熱反應(yīng)器 復(fù)合催化劑 iCWPO UV/Fenton氧化 協(xié)同催化

【摘要】：印染廢水是我國主要有害、難降解的工業(yè)廢水之一。隨著新型助劑、染料等在印染行業(yè)中的大量使用,使染料廢水中的底物不斷向抗光解、抗氧化、抗生物降解方向發(fā)展。目前,處理印染廢水的可行方法包括生物、化學(xué)和物理化學(xué)技術(shù),但傳統(tǒng)的生物化學(xué)法難以得到理想的結(jié)果。近年來,多相催化濕式氧化法因其高效性和穩(wěn)定性具有廣闊的發(fā)展前景,但存在處理成本高、反應(yīng)條件苛刻的缺點(diǎn)。為增強(qiáng)其有效性及實(shí)用性,使發(fā)生條件溫和,研究者添加具有強(qiáng)氧化能力的H2O2作為氧化劑增強(qiáng)處理效果,即催化濕式過氧化氫氧化技術(shù)。催化劑中負(fù)載的活性金屬能夠加速反應(yīng)的進(jìn)行,提高其催化活性、穩(wěn)定性和特定的吸附性能,提高反應(yīng)效率�？蓪煞N或兩種以上金屬溶液混合浸漬,制備復(fù)合金屬氧化物,使催化活性明顯提高,加速催化反應(yīng)的進(jìn)行。磁性或?qū)щ姴牧鲜艿酵饧痈哳l交變磁場(chǎng)作用時(shí)會(huì)感應(yīng)發(fā)熱,鐵磁材料在交變磁場(chǎng)中能夠迅速升溫。我們對(duì)非均相反應(yīng)體系的染料廢水處理進(jìn)行改進(jìn),采用具有較好感應(yīng)熱性能的鐵磁材料或制備具有感應(yīng)內(nèi)核的催化劑,外加全場(chǎng)分布的高頻交變磁場(chǎng)使材料感應(yīng)產(chǎn)熱。通過對(duì)分散的催化劑顆粒增設(shè)感應(yīng)特性,使外部輸入的電磁能量只在顆粒表面實(shí)現(xiàn)熱能轉(zhuǎn)換而不作用于水相,能量的轉(zhuǎn)換更集中于實(shí)際的微觀反應(yīng)位點(diǎn)。本文以碳包覆海綿鐵(SI-C)為載體負(fù)載金屬,制備具有感應(yīng)磁核的多金屬復(fù)合催化劑,實(shí)現(xiàn)感應(yīng)熱反應(yīng)器CWPO(iCWPO)處理低濃度難降解污染物,并結(jié)合紫外光助芬頓反應(yīng)協(xié)同處理高濃度染料廢水。主要結(jié)論如下：(1)以SI-C為載體,Ni的硝酸鹽為前驅(qū)物,采用混合浸漬焙燒法制備了SI-C表層負(fù)載型復(fù)合金屬催化劑(Mn-Ni/C、Mn-La/C、Ni-La/C、Mn-Ni-La/C)。對(duì)催化材料及其前軀體的形貌和結(jié)構(gòu)表征,海綿鐵的主要成分是鐵及鐵的氧化物,具有良好的磁熱效應(yīng)；SI-C表層原子排布緊密,海綿鐵原有的孔隙結(jié)構(gòu)被活性炭層覆蓋,為載體負(fù)載活性金屬提供了條件；負(fù)載型多金屬催化劑表面有光澤,具有明顯分層現(xiàn)象,孔隙分布均勻,有利于進(jìn)行物質(zhì)和能量交換。(2)用Fe/C比4：1反復(fù)包覆海綿鐵3次可實(shí)現(xiàn)較好包覆。0.02 mol/L的La、Mn、Ni硝酸鹽金屬浸漬液以體積比1：1：1均勻混合,并在300。C焙燒2h制得的Mn-Ni-La/C多金屬復(fù)合催化劑具有良好的磁熱效應(yīng)和催化氧化性能。(3)在常溫常壓iCWPO處理低濃度染料廢水工藝中,對(duì)直接藍(lán)D-3GL的去除率達(dá)98.39%,對(duì)直接紫D-BL的去除率達(dá)97.56%,對(duì)直接大紅D-GLN的去除率達(dá)92.18%。表明Mn-Ni-La/C在常溫常壓iCWPO工藝中有較好的催化活性,且反應(yīng)條件溫和,明顯降低了反應(yīng)器液相溫度,促進(jìn)非均相催化反應(yīng)的進(jìn)行。(4)研究了常溫常壓下UV/Mn2+-Fe3+/H2O2光催化均相反應(yīng)體系處理低濃度偶氮染料廢水的特性,紫外光、H202以及金屬離子在均相反應(yīng)體系中具有良好的協(xié)同催化作用。金屬離子在反應(yīng)中起激發(fā)和傳遞作用,使鏈反應(yīng)持續(xù)進(jìn)行直至耗盡H2O2。在20 w紫外光源照射下,Mn2+-Fe3+投加量均為3 mmol,且H2O2投加量為10 ml/L時(shí),直接大紅D-GLN在反應(yīng)20 min時(shí),脫色率就已達(dá)到90%以上。(5)將iCWPO與UV/Mn2+-Fe3+/H2O2反應(yīng)體系結(jié)合,協(xié)同處理高濃度難降解污染物,徹底破壞了染料分子的共軛發(fā)色基團(tuán),并提高廢水的可生化性。在4 w紫外燈照射下,Mn2+-Fe3+投加量均為1 mmol, H2O2投加量為5 ml/L時(shí),600 mg/L的偶氮染料模擬廢水在經(jīng)過光催化反應(yīng)60 min后,通過iCWPO作用,對(duì)直接紫D-BL的脫色率和COD去除率分別為90.46%和80.14%,對(duì)直接藍(lán)D-3GL的處理效率可達(dá)到94.83%和87.53%,對(duì)直接大紅D-GLN的脫色率和COD去除率分別91.35%、82.47%。UV/Mn2+-Fe3+/H2O2反應(yīng)體系與感應(yīng)熱體系的協(xié)同催化作用有效促進(jìn)了非均相催化反應(yīng)的進(jìn)行,使活性金屬高效催化分解H2O2引發(fā)鏈?zhǔn)阶杂苫磻?yīng),破壞染料分子共軛結(jié)構(gòu),實(shí)現(xiàn)高效降解。
[Abstract]:Printing and dyeing wastewater is the main harmful, one of the industrial wastewater is difficult to degrade. With the extensive use of new additives, dyes in the dyeing industry, the dye wastewater substrate to anti photolysis, anti-oxidation, anti biodegradation direction. At present, the methods of dyeing wastewater treatment including biological, chemical and physical chemistry technology, but it is difficult for the traditional biochemical method to get the ideal results. In recent years, multi phase catalytic wet oxidation method for its high efficiency and stability and has broad prospects for development, but there are high cost, harsh reaction conditions and shortcomings. In order to enhance their effectiveness and practicability, the occurrence of mild conditions, the researchers add with the strong oxidation ability of H2O2 as oxidant to enhance the treatment effect, namely the catalytic wet peroxide oxidation technology. The load active metal catalyst can accelerate the reaction, improve its catalytic activity, Stability and specific adsorption performance, improve the reaction efficiency. Can be two or more than two kinds of metal solution impregnation, preparation of composite metal oxides, the catalytic activity increased significantly, to accelerate the catalytic reaction. The magnetic or conductive materials by high frequency alternating magnetic field during induction heating, the ferromagnetic materials can be rapidly warming in the alternating magnetic field. The heterogeneous reaction system in dye wastewater treatment was improved, the catalyst has good thermal properties of ferromagnetic materials of induction or preparation of magnetic core, and the high frequency alternating magnetic field distribution of the material induced heat production. Through the addition of catalyst particle dispersion characteristics of the electromagnetic induction, external energy input only in thermal energy conversion to achieve particle surface rather than the aqueous phase, micro reaction sites of energy conversion is more focused on practical. The carbon coated sponge iron (SI-C) for supported metal, multi metal catalyst preparation with magnetic core, the induction heat CWPO reactor (iCWPO) treating low concentration of refractory pollutants, combined with UV and Fenton reaction synergistic treatment of high concentration dye wastewater. The main conclusions are as follows: (1) based on SI-C and nitrate Ni as the precursor, SI-C surface supported composite catalysts were prepared by impregnation method mixed (Mn-Ni/C, Mn-La/C, Ni-La/C, Mn-Ni-La/C). The morphology and structure characterization of catalytic materials and its precursors, the main component of sponge iron is iron and iron oxide, has good magnetocaloric effect; SI-C surface atomic arrangement close the pore structure of the sponge iron original activated carbon layer, provides conditions for the carrier to load active metal supported multi metal catalyst; surface luster, has obvious stratification phenomenon, uniform pore distribution is Conducive to the exchange of material and energy. (2) by Fe/C 4:1 coated sponge iron 3 times repeatedly can achieve better.0.02 mol/L coated La, Mn, Ni metal nitrate solution with the volume ratio of 1:1:1 mixture, and has the magnetocaloric effect and good catalytic performance in 300.C roasting 2H prepared Mn-Ni-La/C multi metal composite catalyst. (3) in normal temperature treatment of low concentration iCWPO dye wastewater, the removal rate of 98.39% direct blue D-3GL, direct violet D-BL on the removal rate of 97.56%, the direct red D-GLN and the removal rate of 92.18%. showed that Mn-Ni-La/C had good catalytic activity in normal temperature and pressure in the iCWPO process, and mild reaction conditions, significantly reduces the temperature of the liquid phase reactor, promote heterogeneous catalytic reaction. (4) studied under normal temperature and pressure UV/Mn2+-Fe3+/H2O2 photocatalytic characteristics of homogeneous reaction system for treatment of low concentration of azo dye wastewater, UV, H202 and metal ions in a homogeneous reaction system has good synergistic catalytic effect. Metal ion excitation and transfer function in the reaction, the chain reaction continues until exhausted by H2O2. in 20 W under irradiation of ultraviolet light, Mn2+-Fe3+ dosage was 3 mmol, and the dosage of H2O2 is 10 ml/L when the direct red D-GLN in the reaction of 20 min, the decolorization rate reached above 90%. (5) the combination of iCWPO and UV/Mn2+-Fe3+/H2O2 reaction system, CO treatment of high concentration refractory pollutants, completely destroyed the conjugate dye molecules chromophore, and improve the biodegradability of waste water. In 4 W UV lamp under the irradiation of Mn2+-Fe3+ dosage was 1 mmol, H2O2 dosage is 5 ml/L, 600 mg/L of azo dye wastewater after photocatalytic reaction after 60 min, the iCWPO effect on direct violet D-BL decolorization and COD removal rates were 90.46% and 80.14%, the The treatment efficiency of direct blue D-3GL can reach 94.83% and 87.53%, of direct red D-GLN decolorization rate and COD removal rate of 91.35%, the synergistic catalytic effect of 82.47%.UV/Mn2+-Fe3+/H2O2 reaction system and induction heat system effectively promoted by heterogeneous catalytic reaction, the catalytic decomposition of H2O2 active metal, initiate free radical chain reaction, destroy the conjugation the structure of dye molecules, achieve high efficiency degradation.

【學(xué)位授予單位】：陜西師范大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：X791

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