本文關(guān)鍵詞：吸波材料與微波輻射協(xié)同降解染料的過程與機(jī)制研究　出處：《遼寧大學(xué)》2016年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 吸波材料 微波照射 染料 降解 鐵氧體

【摘要】：近年來,隨著經(jīng)濟(jì)的快速發(fā)展,人類對(duì)環(huán)境的重視度越來越高。而在環(huán)境污染中,大部分直接與工業(yè)和工業(yè)產(chǎn)品的污染有關(guān)。多數(shù)染料及染料中間體都具有致癌、致畸、致突變效應(yīng),生物毒性大的特點(diǎn),對(duì)人類的健康和生態(tài)系統(tǒng)都造成嚴(yán)重的危害。探索染料的降解方法,已經(jīng)成為當(dāng)務(wù)之急。本論文研究了自制吸波材料AB204(A=Sr,Ba,Fe,B=Fe,Co)作為催化劑,微波照射協(xié)同作用(MW/AB2O4)降解染料廢水(結(jié)晶紫、甲基紫、孔雀綠)的作用效果,考察了AB204的煅燒溫度、染料初始濃度、催化劑加入量、染料溶液的pH值、微波輸出功率、微波輻射時(shí)間、干擾離子等因素對(duì)降解效率的影響,確定了實(shí)驗(yàn)的最佳條件,并通過一系列的分析方法對(duì)AB204的降解機(jī)理進(jìn)行揭示。采用溶膠-凝膠(sol-gel)法合成磁性鐵氧體SrFe2O4,并用XRD,SEM和VSM等方法對(duì)所得SrFe2O4進(jìn)行表征,結(jié)果表明制得尖晶石結(jié)構(gòu)的SrFe2O4,并且具有很好的磁性。選擇染料污染物-結(jié)晶紫和甲基紫為目標(biāo)污染物,研究MW/SrFe2O4體系對(duì)結(jié)晶紫和甲基紫的降解效果。MW/SrFe2O4協(xié)同降解染料的最佳降解條件為：SrFe2O4的煅燒溫度是400℃,加入SrFe2O4的質(zhì)量分?jǐn)?shù)為0.1%,對(duì)50 mL 10 mg L-1的結(jié)晶紫和甲基紫溶液在微波輸出功率500 W,微波輻射8 min后的降解效率能達(dá)到80%以上。降解動(dòng)力學(xué)實(shí)驗(yàn)結(jié)果表明：MW/SrFe2O4協(xié)同降解結(jié)晶紫／甲基紫反應(yīng)符合準(zhǔn)一級(jí)動(dòng)力學(xué)模型,反應(yīng)速率常數(shù)分別為0.22 min-1和0.17 mmin-1。采用自由基捕獲實(shí)驗(yàn)和熒光實(shí)驗(yàn)的方法得出MW/SrFe2O4協(xié)同降解結(jié)晶紫和甲基紫的實(shí)驗(yàn)過程中,產(chǎn)生的活性物質(zhì)主要是超氧自由基,空穴和羥自由基。它們能夠氧化染料,使染料快速降解成對(duì)環(huán)境無害的無機(jī)離子。采用檸檬酸鹽-硝酸鹽燃燒法合成磁性鐵氧體BaFe2O4,并用XRD,SEM和VSM等方法對(duì)所得BaFe2O4進(jìn)行表征,結(jié)果表明制得尖晶石結(jié)構(gòu)的BaFe2O4,并且具有很好的磁性。選擇染料污染物-結(jié)晶紫為目標(biāo)污染物,研究MW/BaFe2O4體系對(duì)結(jié)晶紫的降解效果。MW/BaFe2O4協(xié)同降解結(jié)晶紫的最佳降解條件為：BaFe2O4的煅燒溫度是800℃,加入BaFe2O4的質(zhì)量分?jǐn)?shù)為0.06%,對(duì)50 mL 10mg L-1的結(jié)晶紫溶液在微波輸出功率500 W,微波輻射8min后的降解效率能達(dá)到90%。降解動(dòng)力學(xué)實(shí)驗(yàn)結(jié)果表明：MW/BaFe2O4協(xié)同降解結(jié)晶紫反應(yīng)符合準(zhǔn)一級(jí)動(dòng)力學(xué)模型,反應(yīng)速率常數(shù)可達(dá)到0.44 min-1。采用自由基捕獲方法得出MW/BaFe2O4協(xié)同降解結(jié)晶紫的實(shí)驗(yàn)過程中,產(chǎn)生的活性物質(zhì)主要是超氧自由基和空穴。它們能夠氧化染料,使染料快速降解成對(duì)環(huán)境無害的C02,H20和一些無機(jī)離子。采用熱分解法合成磁性鐵氧體FeCo2O4,并用XRD,SEM和VSM等方法對(duì)所得FeCo2O4進(jìn)行表征,結(jié)果表明制得尖晶石結(jié)構(gòu)的FeCo2O4,并且具有很好的磁性。選擇染料污染物一孔雀綠為目標(biāo)污染物,研究MW/FeCo2O4體系對(duì)孔雀綠的降解效果。MW/FeCo2O4協(xié)同降解孔雀綠的最佳降解條件為：FeCo2O4的煅燒溫度是600℃,加入FeCo2O4的質(zhì)量分?jǐn)?shù)為0.2%,對(duì)50 mL 20 mg L-1的孔雀綠溶液在微波輸出功率500 W,微波輻射8 min后的降解效率能達(dá)到90%。降解動(dòng)力學(xué)實(shí)驗(yàn)結(jié)果表明：MW/FeCo2O4協(xié)同降解結(jié)晶紫反應(yīng)符合準(zhǔn)一級(jí)動(dòng)力學(xué)模型,反應(yīng)速率常數(shù)可達(dá)到0.13 min-1。采用自由基捕獲實(shí)驗(yàn)得出MW/FeCo2O4協(xié)同降解孔雀綠的實(shí)驗(yàn)過程中,產(chǎn)生的活性物質(zhì)主要是超氧自由基和空穴。它們能夠氧化染料,使染料快速降解成對(duì)環(huán)境無害的CO2,H2O和一些無機(jī)離子。結(jié)果研究表明,MW/AB2O4協(xié)同作用降解染料,從傳統(tǒng)的幾個(gè)小時(shí),縮短到現(xiàn)在的幾分鐘,大大縮短了降解時(shí)間,提高了降解速率。此外通過離子色譜、紫外測(cè)定結(jié)果可知,難降解的染料有機(jī)分子已被完全礦化為無機(jī)離子等無害物質(zhì),幾乎沒有中間產(chǎn)物產(chǎn)生,不會(huì)造成二次污染。同時(shí)通過外加磁場(chǎng)可將AB204進(jìn)行回收利用,而且催化劑的循環(huán)利用次數(shù)達(dá)到四次后的降解效率依然在80%以上,減少了資源的浪費(fèi),減少了對(duì)生態(tài)環(huán)境的破壞。
[Abstract]:In recent years, with the rapid development of economy, human beings on the environment are paying more and more attention. In environmental pollution, the most direct and industrial products and industrial pollution. The majority of dyes and dye intermediates are carcinogenic, teratogenic, mutagenic effect, characteristics of biological toxicity, causing serious harm to human the health and ecological system. To explore the degradation methods of dyes, has become a pressing matter of the moment. This paper studies the self-made microwave absorbing materials AB204 (A=Sr, Ba, Fe, B=Fe, Co) as catalyst, microwave irradiation synergy (MW/AB2O4) degradation of dye wastewater (crystal violet, methyl violet, malachite green) effect was investigated the calcination temperature of AB204, initial dye concentration, catalyst dosage, pH value of dye solution, microwave power, microwave radiation time, interfering ions and other factors on the degradation efficiency of the influence, determine the optimal experimental conditions, and through The degradation mechanism analysis of a series of methods of AB204 are revealed. By using sol gel (sol-gel) method for the synthesis of magnetic ferrite SrFe2O4, and XRD, SEM and VSM methods were used to characterize the obtained SrFe2O4, results show that the prepared spinel structure of SrFe2O4, and has a very good choice. The magnetic dye pollutants - crystallization purple and violet as the target pollutant, the optimal degradation conditions of.MW/SrFe2O4 degradation effects of MW/SrFe2O4 system on crystal violet and violet synergistic degradation of dyes as the calcination temperature of SrFe2O4 is 400 DEG C, concentration of SrFe2O4 was 0.1%, 50 mL 10 mg L-1 crystal violet and methyl violet solution in the microwave output power is 500 W, degradation the efficiency of 8 min after microwave radiation can reach more than 80%. The experimental results show that the degradation kinetics of MW/SrFe2O4 synergetic degradation of crystal violet / methyl violet was consistent with pseudo first order kinetic model of reaction The rate constants were 0.22 min-1 and 0.17 mmin-1. by free radical trapping experiments and fluorescence experiments that MW/SrFe2O4 co degradation of crystal violet and violet in the main active substance is produced superoxide radical, hydroxyl radical and hole. They can oxidation dyes, inorganic ion dye fast degradation into nontoxic. Using citrate nitrate combustion synthesis of magnetic ferrite and BaFe2O4, XRD, SEM and VSM methods were used to characterize the obtained BaFe2O4, results show that the prepared spinel structure of BaFe2O4, and has a very good choice. The magnetic crystal violet dye pollutants as the target pollutant, the degradation effect of crystal violet on.MW/BaFe2O4 the MW/BaFe2O4 system of the synergistic degradation of crystal violet for optimal degradation conditions: the calcination temperature of BaFe2O4 is 800 DEG C, concentration of BaFe2O4 is 0.06% to 50, mL 10mg Crystal violet solution L-1 in the microwave output power of 500 W, the degradation rate of 8min after microwave radiation can reach the experimental results of 90%. degradation kinetics showed that MW/BaFe2O4 co degradation of crystal violet was consistent with pseudo first order kinetic model, the reaction rate constant can reach 0.44 min-1. by free radical trapping method to obtain the MW/BaFe2O4 synergistic degradation of crystal violet in the course of the experiments. The main active substance is produced superoxide radical and hole. They can make rapid degradation of oxidation dyes, dye into nontoxic C02, H20 and some inorganic ions. The decomposition of magnetic ferrite and FeCo2O4, XRD, SEM and VSM were used to the FeCo2O4, the results show that the as prepared the spinel structure of FeCo2O4, and has a good selection of magnetic. A malachite green dye pollutants as target pollutants, research on the system of MW/FeCo2O4 effect on the degradation of malachite green. The optimal degradation conditions of MW/FeCo2O4 synergetic degradation of malachite green as the calcination temperature of FeCo2O4 is 600 DEG C, concentration of FeCo2O4 was 0.2%, 50 mL 20 mg malachite green solution on L-1 in the microwave output power is 500 W, can reach 90%. degradation dynamics experimental results show that the degradation rate of 8 min after microwave radiation: MW/FeCo2O4 synergistic degradation of Crystal Purple was consistent with pseudo first order kinetic model, the reaction rate constant can reach 0.13 min-1. capture experiment of MW/FeCo2O4 synergetic degradation of malachite green by free radical, the main active substances are produced superoxide radical and hole. They can make rapid degradation of oxidation dyes, dye into nontoxic CO2, H2O and some inorganic ions. The results of study showed that the synergetic effect of MW/AB2O4 degradation, from a few hours to traditional, now shortened to a few minutes, greatly shorten the time of degradation. The high rate of degradation. The results showed that ion chromatography, UV dye, organic molecules refractory has been completely mineralized to inorganic ions and other harmful substances, almost no intermediate products produced, will not cause two pollution. At the same time by the external magnetic field AB204 can be recycled, and the number of recycling catalyst to degrade after four times the efficiency was still above 80%, reduce the waste of resources, reduce the damage to the ecological environment.

【學(xué)位授予單位】：遼寧大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2016
【分類號(hào)】：X788;O643.36

【參考文獻(xiàn)】

相關(guān)期刊論文 前1條

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本文編號(hào)：1413989