濕式過(guò)氧化氫氧化活性艷藍(lán)KN-R的實(shí)驗(yàn)研究及機(jī)理分析
發(fā)布時(shí)間：2018-12-25 12:06
【摘要】：隨著印染行業(yè)的發(fā)展,染料廢水對(duì)水體的污染日益嚴(yán)重。由于染料廢水中含有大量的、難以被微生物降解的有毒有害物質(zhì),使印染廢水的污染治理成為人們關(guān)注的焦點(diǎn)。在所有染料中,蒽醌染料的使用量?jī)H次于偶氮染料。由于其具有十分穩(wěn)定的蒽醌結(jié)構(gòu),不易被生物降解,因而在環(huán)境中殘留時(shí)間長(zhǎng)�；钚云G藍(lán)KN-R是一種典型的蒽醌類染料。為了有效地處理印染廢水,本論文采用了濕式過(guò)氧化氫氧化法(Wet Peroxide Oxidation,簡(jiǎn)稱WPO)降解活性艷藍(lán)KN-R。通過(guò)篩選反應(yīng)因子,獲得最佳的條件是:H_2O_2的添加劑量為20.4μL,即反應(yīng)體系中H_2O_2的溶度為0.01 mol/L,反應(yīng)溫度為150°C,反應(yīng)時(shí)間為4 h,反應(yīng)壓強(qiáng)為0.5 MPa,p H為6.8。在最佳的條件下處理后,活性艷藍(lán)KN-R模擬廢水的顏色由深藍(lán)色變?yōu)闊o(wú)色。當(dāng)初始濃度為200 mg/L時(shí),在最優(yōu)條件下,活性艷藍(lán)KN-R的脫色率和TOC去除率分別為100%和68.54%。在120~150°C范圍內(nèi)考察了該反應(yīng)的動(dòng)力學(xué),結(jié)果表明活性艷藍(lán)KN-R的濕式過(guò)氧化氫氧化反應(yīng)符合準(zhǔn)一級(jí)動(dòng)力學(xué)方程,并且通過(guò)計(jì)算得到了反應(yīng)活化能為73.9 k J/mol(R2=0.96)。對(duì)活性艷藍(lán)KN-R經(jīng)WPO法降解后的產(chǎn)物,利用氣相色譜/質(zhì)譜聯(lián)用儀(GC-MS)進(jìn)行鑒定。結(jié)果表明其降解產(chǎn)物主要為小分子有機(jī)酸,如丁二酸、已二酸、鄰苯二甲酸,而這種小分子酸都是可生化的,這說(shuō)明經(jīng)過(guò)WPO降解后,活性艷藍(lán)KN-R的可生化性有所提高。通過(guò)添加自由基捕獲劑(叔丁醇)研究了自由基反應(yīng)機(jī)理,結(jié)果顯示,自由基捕獲劑的存在對(duì)WPO法降解活性艷藍(lán)KN-R有負(fù)面影響。150°C,0.5 MPa氧氣壓力,加入叔丁醇,反應(yīng)4 h后,溶液在596 nm處的吸光度從0.00725增加到0.40696,因此H_2O_2在反應(yīng)過(guò)程中產(chǎn)生了羥基自由基,并且高反應(yīng)活性的羥基自由基也參與了WPO法降解活性艷藍(lán)KN-R的反應(yīng)機(jī)制。
[Abstract]:With the development of printing and dyeing industry, dye wastewater pollution to water is becoming more and more serious. Because dye wastewater contains a lot of toxic and harmful substances which are difficult to be degraded by microorganisms, the pollution treatment of printing and dyeing wastewater has become the focus of attention. Of all the dyes, anthraquinone dyes are used second only to azo dyes. Because of its stable anthraquinone structure, it is difficult to biodegrade, so it remains in the environment for a long time. Reactive brilliant blue KN-R is a typical anthraquinone dye. In order to deal with printing and dyeing wastewater effectively, wet hydrogen peroxide oxidation (Wet Peroxide Oxidation,) method was used to degrade reactive brilliant blue KN-R. (WPO). By screening the reaction factors, the optimum conditions were obtained as follows: the amount of H_2O_2 was 20.4 渭 L, that is, the solubility of H_2O_2 in the reaction system was 0. 01 mol/L, the reaction temperature was 150 擄C, the reaction time was 4 h. The reaction pressure is 0. 5 MPa,p H is 6. 8. After treatment under the best conditions, the color of reactive brilliant blue KN-R simulated wastewater changed from dark blue to colorless. When the initial concentration was 200 mg/L, the decolorization and TOC removal rates of reactive brilliant blue KN-R were 100% and 68.54%, respectively. The kinetics of the reaction was investigated in the range of 120 擄C. The results show that the wet hydrogen peroxide oxidation reaction of reactive brilliant blue KN-R accords with the quasi first-order kinetic equation, and the activation energy of the reaction is 73.9 k J/mol (R20.96). The products of reactive brilliant blue KN-R degraded by WPO were identified by gas chromatography / mass spectrometry (GC-MS). The results showed that the degradation products were mainly small molecular organic acids, such as succinic acid, adipic acid and phthalic acid, which were biodegradable, which indicated that the biodegradability of reactive brilliant blue KN-R was improved after WPO degradation. The mechanism of free radical reaction was studied by adding free radical trapping agent (tert-butanol). The results showed that the existence of free radical trapping agent had a negative effect on the degradation of reactive brilliant blue KN-R by WPO method. After 4 h reaction, the absorbance of the solution at 596 nm increased from 0.00725 to 0.40696, so H_2O_2 produced hydroxyl radical during the reaction. The hydroxyl radical with high reactive activity also participated in the degradation mechanism of reactive brilliant blue KN-R by WPO method.
【學(xué)位授予單位】：湖南大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：X791
[Abstract]:With the development of printing and dyeing industry, dye wastewater pollution to water is becoming more and more serious. Because dye wastewater contains a lot of toxic and harmful substances which are difficult to be degraded by microorganisms, the pollution treatment of printing and dyeing wastewater has become the focus of attention. Of all the dyes, anthraquinone dyes are used second only to azo dyes. Because of its stable anthraquinone structure, it is difficult to biodegrade, so it remains in the environment for a long time. Reactive brilliant blue KN-R is a typical anthraquinone dye. In order to deal with printing and dyeing wastewater effectively, wet hydrogen peroxide oxidation (Wet Peroxide Oxidation,) method was used to degrade reactive brilliant blue KN-R. (WPO). By screening the reaction factors, the optimum conditions were obtained as follows: the amount of H_2O_2 was 20.4 渭 L, that is, the solubility of H_2O_2 in the reaction system was 0. 01 mol/L, the reaction temperature was 150 擄C, the reaction time was 4 h. The reaction pressure is 0. 5 MPa,p H is 6. 8. After treatment under the best conditions, the color of reactive brilliant blue KN-R simulated wastewater changed from dark blue to colorless. When the initial concentration was 200 mg/L, the decolorization and TOC removal rates of reactive brilliant blue KN-R were 100% and 68.54%, respectively. The kinetics of the reaction was investigated in the range of 120 擄C. The results show that the wet hydrogen peroxide oxidation reaction of reactive brilliant blue KN-R accords with the quasi first-order kinetic equation, and the activation energy of the reaction is 73.9 k J/mol (R20.96). The products of reactive brilliant blue KN-R degraded by WPO were identified by gas chromatography / mass spectrometry (GC-MS). The results showed that the degradation products were mainly small molecular organic acids, such as succinic acid, adipic acid and phthalic acid, which were biodegradable, which indicated that the biodegradability of reactive brilliant blue KN-R was improved after WPO degradation. The mechanism of free radical reaction was studied by adding free radical trapping agent (tert-butanol). The results showed that the existence of free radical trapping agent had a negative effect on the degradation of reactive brilliant blue KN-R by WPO method. After 4 h reaction, the absorbance of the solution at 596 nm increased from 0.00725 to 0.40696, so H_2O_2 produced hydroxyl radical during the reaction. The hydroxyl radical with high reactive activity also participated in the degradation mechanism of reactive brilliant blue KN-R by WPO method.
【學(xué)位授予單位】：湖南大學(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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