超声/Fe~0/EDTA体系对印染污泥中多环芳烃的降解
|
摘要
Fe~0/EDTA类芬顿体系能产生氧化能力极强的羟基自由基(·OH),已被广泛应用于有机污染物的去除.提高·OH的生成速率和浓度是高效降解有机污染物的关键.因此,本文利用超声/Fe~0/EDTA体系处理印染污泥,探讨了不同反应参数对体系中产生·OH的影响,考察了该体系对印染污泥中多环芳烃(PAHs)的去除效果.结果表明,在pH为3.0,超声功率为540 W,Fe~0投加量为15 g·L~(-1),EDTA浓度为2.0 mmol·L~(-1)的最佳条件下,·OH浓度高达862μmol·L~(-1).印染污泥中的铁絮凝剂可作为超声/Fe~0/EDTA体系中Fe~(2+)和Fe~(3+)的来源,促使该体系循环产生H_2O_2和·OH.超声/Fe~0/EDTA体系产生的·OH能快速有效地降解印染污泥中的PAHs,∑_(16)PAHs的平均去除率达到77%,同时有机质含量下降了10.1%.
The Fe~0/EDTA Fenton like system could produce hydroxyl radicals( ·OH) which possesses strong oxidizing capacity,and was widely used for the removal of organic pollutants. Increasing the generation rate and concentration of ·OH was the key step for the efficient degradation of organic pollutants. An ultrasound/Fe~0/EDTA system was proposed for generating ·OH and removing polycyclic aromatic hydrocarbons( PAHs) from textile dyeing sludge. Effect of reaction parameters on ·OH production and resultant degradation of PAHs were examined. Results indicated that the ultrasound/Fe~0/EDTA system can produce high concentration of ·OH up to 862 μmol·L~(-1) at pH 3. 0,ultrasonic power of 500 W,Fe~0 dosages of 15 g·L~(-1) and EDTA concentration of 2. 0 mmol·L~(-1). Iron flocculant remaining in textile dyeing sludge was an important source of Fe~(2+)and Fe~(3+),promoting the spontaneous generation of H_2O_2 and ·OH in the ultrasound/Fe~0/EDTA system. The PAHs in textile dyeing sludge can be quickly and effectively degraded by the ·OH generated by the ultrasound/Fe~0/EDTA system,with an average removal efficiency of 77% for ∑_(16)PAHs,and was companied by 10.1% decreases in organic matter content.
The Fe~0/EDTA Fenton like system could produce hydroxyl radicals( ·OH) which possesses strong oxidizing capacity,and was widely used for the removal of organic pollutants. Increasing the generation rate and concentration of ·OH was the key step for the efficient degradation of organic pollutants. An ultrasound/Fe~0/EDTA system was proposed for generating ·OH and removing polycyclic aromatic hydrocarbons( PAHs) from textile dyeing sludge. Effect of reaction parameters on ·OH production and resultant degradation of PAHs were examined. Results indicated that the ultrasound/Fe~0/EDTA system can produce high concentration of ·OH up to 862 μmol·L~(-1) at pH 3. 0,ultrasonic power of 500 W,Fe~0 dosages of 15 g·L~(-1) and EDTA concentration of 2. 0 mmol·L~(-1). Iron flocculant remaining in textile dyeing sludge was an important source of Fe~(2+)and Fe~(3+),promoting the spontaneous generation of H_2O_2 and ·OH in the ultrasound/Fe~0/EDTA system. The PAHs in textile dyeing sludge can be quickly and effectively degraded by the ·OH generated by the ultrasound/Fe~0/EDTA system,with an average removal efficiency of 77% for ∑_(16)PAHs,and was companied by 10.1% decreases in organic matter content.
引文
曹梦华.2013.基于零价铁的复合污染土壤化学修复研究[D].武汉:华中科技大学.20-53
Fu D M,Messele S A,Fortuny A,et al.2015.Efficient elimination of tyrosol in a zero valent iron-EDTA system at mild conditions[J].Chemical Engineering Journal,260:199-208
Gogate P R,Pandit A B.2004.A review of imperative technologies for wastewater treatment I:oxidation technologies at ambient conditions[J].Advances in Environmental Research,8(3/4):501-551
Harrison E Z,Oakes S R,Hysell M,et al.2006.Organic chemicals in sewage sludges[J].Science of the Total Environment,367(2/3):481-497
Harvey A E J,Smart J A,Amis E S.1955.Simultaneous spectrophotometric determination of iron(II)and total iron with 1,10-phenanthroline[J].Analytical Chemistry,27(1):26-29
Ibá1ez G R,Esteban B,Ponce-Robles L,et al.2015.Fate of micropollutants during sewage sludge disintegration by low-frequency ultrasound[J].Chemical Engineering Journal,280:575-587
Ikai H,Nakamura K,Shirato M,et al.2010.Photolysis of hydrogen peroxide,an effective disinfection system via hydroxyl radical formation[J].Antimicrobial Agents Chemotherapy,54(12):5086-5091
Iwamori S,Nishiyama N,Oya K.2016.A colorimetric indicator for detection of hydroxyl radicals in atmosphere using a methylene blue dye based on nafionfilm[J].Polymer Degradation and Stability,123(38):131-136
Keenan C R,Sedlak D L.2008.Ligand-enhanced reactive oxidant generation by nanoparticulate zero-valent iron and oxygen[J].Environmental Science&Technology,42(18):6936-6941
Kwon B G,Dong S L,Kang N,et al.1999.Characteristics of pchlorophenol oxidation by Fenton's reagant[J].Water Research,33(9):2110-2118
李海静.2012.絮凝剂处理污水的现状及对策研究[J].环境保护与循环经济,(6):53-56
Lindsey M E,Tarr M A.2000.Quantitation of hydroxyl radical during Fenton oxidation following a single addition of iron and peroxide[J].Chemosphere,41:409-417
Lin M Q,Ning X A,An T C,et al.2016.Degradation of polycyclic aromatic hydrocarbons(PAHs)in textile dyeing sludge with ultrasound and Fenton processes:Effect of system parameters and synergistic effect study[J].Journal of Hazardous Materials,307:7-16
Liu B,Li S,Zhao Y,et al.2010.Enhanced degradation of 4-nitrophenol by microwave assisted Fe/EDTA process[J].Journal of Hazardous Materials,176(1):213-219
Lu M,Wei X F.2011.Treatment of oilfield wastewater containing polymer by the batch activated sludge reactor combined with a zero valent iron/EDTA/air system[J].Bioresource Technology,102(3):2555-2562
Maezono T,Tokumura M,Sekine M,et al.2011.Hydroxyl radical concentration profile in photo-Fenton oxidation process:Generation and consumption of hydroxyl radicals during the discoloration of azodye Orange II[J].Chemosphere,82(10):1422-1430
Ning X A,Lin M Q,Shen L Z,et al.2014.Levels,composition profiles and risk assessment of polycyclic aromatic hydrocarbons(PAHs)in sludge from ten textile dyeing plants[J].Environmental Research,132:112-118
Noradoun C E,Cheng I F.2005.EDTA degradation induced by oxygen activation in a zero valent iron/air/water system[J].Environmental Science&Technology,39(18):7158-7163
Oh J Y,Choi S D,Kwon H O,et al.2016.Leaching of polycyclic aromatic hydrocarbons(PAHs)from industrial wastewater sludge by ultrasonic treatment[J].Ultrasonics Sonochemistry,33:61-66
Ranc B,Faure P,Croze V,et al.2016.Selection of oxidant doses for in situ chemical oxidation of soils contaminated by polycyclic aromatic hydrocarbons(PAHs):A review[J].Journal of Hazardous Materials,312:280-297
Rose A L,Waite T D.2002.Kinetic model for Fe(II)oxidation in seawater in the absence and presence of natural organic matter[J].Environmental Science&Technology,36(3):433-444
Seibig S,Eldik R V.1997.Kinetics of[FeII(edta)]oxidation by molecular oxygen revisited.New evidence for a multistep mechanism[J].Inorganic Chemistry,36(18):4115-4120
Tokumura M,Morito R,Hatayama R,et al.2011.Iron redox cycling in hydroxyl radical generation during the photo-Fenton oxidative degradation:Dynamic change of hydroxyl radical concentration[J].Applied Catalysis B Environmental,106(3/4):565-576
Wang A M,Li Y Y,Ru J.2010.The mechanism and application of the Electro-Fenton process for azo dye Acid Red 14 degradation using an activated carbon fibre felt cathode[J].Journal of Chemical Technology&Biotechnology,85(11):1463-1470
杨春维,王栋,郭建博,等.2006.水中有机物高级氧化过程中的羟基自由基检测方法比较[J].环境污染治理技术与设备,7(1):136-141
Zeng Q,Dong H,Wang X,et al.2017.Degradation of 1,4-dioxane by hydroxyl radicals produced from clay minerals[J].Journal of Hazardous Materials,331:88-89
Zhou H Y,Sun Q,Wang X,et al.2014.Removal of 2,4-dichlorophenol from contaminated soil by a heterogeneous ZVI/EDTA/Air Fentonlike system[J].Separation and Purification Technology,132:346-353
Zhou T,Lim T T,Lu X H,et al.2009.Simultaneous degradation of 4CPand EDTA in a heterogeneous Ultrasound/Fenton like system at ambient circumstance[J].Separation and Purification Technology,68(3):367-374
Zhou T,Lim T T,Li Y Z,et al.2010.The role and fate of EDTA in ultrasound-enhanced zero-valent iron/air system[J].Chemosphere,78(5):576-582
Fu D M,Messele S A,Fortuny A,et al.2015.Efficient elimination of tyrosol in a zero valent iron-EDTA system at mild conditions[J].Chemical Engineering Journal,260:199-208
Gogate P R,Pandit A B.2004.A review of imperative technologies for wastewater treatment I:oxidation technologies at ambient conditions[J].Advances in Environmental Research,8(3/4):501-551
Harrison E Z,Oakes S R,Hysell M,et al.2006.Organic chemicals in sewage sludges[J].Science of the Total Environment,367(2/3):481-497
Harvey A E J,Smart J A,Amis E S.1955.Simultaneous spectrophotometric determination of iron(II)and total iron with 1,10-phenanthroline[J].Analytical Chemistry,27(1):26-29
Ibá1ez G R,Esteban B,Ponce-Robles L,et al.2015.Fate of micropollutants during sewage sludge disintegration by low-frequency ultrasound[J].Chemical Engineering Journal,280:575-587
Ikai H,Nakamura K,Shirato M,et al.2010.Photolysis of hydrogen peroxide,an effective disinfection system via hydroxyl radical formation[J].Antimicrobial Agents Chemotherapy,54(12):5086-5091
Iwamori S,Nishiyama N,Oya K.2016.A colorimetric indicator for detection of hydroxyl radicals in atmosphere using a methylene blue dye based on nafionfilm[J].Polymer Degradation and Stability,123(38):131-136
Keenan C R,Sedlak D L.2008.Ligand-enhanced reactive oxidant generation by nanoparticulate zero-valent iron and oxygen[J].Environmental Science&Technology,42(18):6936-6941
Kwon B G,Dong S L,Kang N,et al.1999.Characteristics of pchlorophenol oxidation by Fenton's reagant[J].Water Research,33(9):2110-2118
李海静.2012.絮凝剂处理污水的现状及对策研究[J].环境保护与循环经济,(6):53-56
Lindsey M E,Tarr M A.2000.Quantitation of hydroxyl radical during Fenton oxidation following a single addition of iron and peroxide[J].Chemosphere,41:409-417
Lin M Q,Ning X A,An T C,et al.2016.Degradation of polycyclic aromatic hydrocarbons(PAHs)in textile dyeing sludge with ultrasound and Fenton processes:Effect of system parameters and synergistic effect study[J].Journal of Hazardous Materials,307:7-16
Liu B,Li S,Zhao Y,et al.2010.Enhanced degradation of 4-nitrophenol by microwave assisted Fe/EDTA process[J].Journal of Hazardous Materials,176(1):213-219
Lu M,Wei X F.2011.Treatment of oilfield wastewater containing polymer by the batch activated sludge reactor combined with a zero valent iron/EDTA/air system[J].Bioresource Technology,102(3):2555-2562
Maezono T,Tokumura M,Sekine M,et al.2011.Hydroxyl radical concentration profile in photo-Fenton oxidation process:Generation and consumption of hydroxyl radicals during the discoloration of azodye Orange II[J].Chemosphere,82(10):1422-1430
Ning X A,Lin M Q,Shen L Z,et al.2014.Levels,composition profiles and risk assessment of polycyclic aromatic hydrocarbons(PAHs)in sludge from ten textile dyeing plants[J].Environmental Research,132:112-118
Noradoun C E,Cheng I F.2005.EDTA degradation induced by oxygen activation in a zero valent iron/air/water system[J].Environmental Science&Technology,39(18):7158-7163
Oh J Y,Choi S D,Kwon H O,et al.2016.Leaching of polycyclic aromatic hydrocarbons(PAHs)from industrial wastewater sludge by ultrasonic treatment[J].Ultrasonics Sonochemistry,33:61-66
Ranc B,Faure P,Croze V,et al.2016.Selection of oxidant doses for in situ chemical oxidation of soils contaminated by polycyclic aromatic hydrocarbons(PAHs):A review[J].Journal of Hazardous Materials,312:280-297
Rose A L,Waite T D.2002.Kinetic model for Fe(II)oxidation in seawater in the absence and presence of natural organic matter[J].Environmental Science&Technology,36(3):433-444
Seibig S,Eldik R V.1997.Kinetics of[FeII(edta)]oxidation by molecular oxygen revisited.New evidence for a multistep mechanism[J].Inorganic Chemistry,36(18):4115-4120
Tokumura M,Morito R,Hatayama R,et al.2011.Iron redox cycling in hydroxyl radical generation during the photo-Fenton oxidative degradation:Dynamic change of hydroxyl radical concentration[J].Applied Catalysis B Environmental,106(3/4):565-576
Wang A M,Li Y Y,Ru J.2010.The mechanism and application of the Electro-Fenton process for azo dye Acid Red 14 degradation using an activated carbon fibre felt cathode[J].Journal of Chemical Technology&Biotechnology,85(11):1463-1470
杨春维,王栋,郭建博,等.2006.水中有机物高级氧化过程中的羟基自由基检测方法比较[J].环境污染治理技术与设备,7(1):136-141
Zeng Q,Dong H,Wang X,et al.2017.Degradation of 1,4-dioxane by hydroxyl radicals produced from clay minerals[J].Journal of Hazardous Materials,331:88-89
Zhou H Y,Sun Q,Wang X,et al.2014.Removal of 2,4-dichlorophenol from contaminated soil by a heterogeneous ZVI/EDTA/Air Fentonlike system[J].Separation and Purification Technology,132:346-353
Zhou T,Lim T T,Lu X H,et al.2009.Simultaneous degradation of 4CPand EDTA in a heterogeneous Ultrasound/Fenton like system at ambient circumstance[J].Separation and Purification Technology,68(3):367-374
Zhou T,Lim T T,Li Y Z,et al.2010.The role and fate of EDTA in ultrasound-enhanced zero-valent iron/air system[J].Chemosphere,78(5):576-582