微波强化铁碳-双氧水体系处理填埋场渗滤液膜滤浓缩液研究
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摘要
为了探讨微波(MW)/铁碳(Fe-C)/H_2O_2类芬顿反应对填埋场渗滤液膜滤浓缩液(简称"渗滤液浓缩液")中难降解有机物,系统研究了双氧水投量、Fe-C投量、初始pH值、微波输出功率和反应时间对浓缩液中有机污染物的去除规律,通过类比实验研究了MW/Fe-C/H_2O_2体系的反应协同作用;此外,采用紫外-可见和三维荧光光谱表征了浓缩液中溶解性有机物的分子结构变化;最后,利用SEM-EDS和XRD等表征对反应前后的Fe-C材料的催化机理进行了解析.结果表明,在双氧水投量为10 mL·L~(-1),Fe-C投量0.8 g·L~(-1),初始pH值为3,微波输出功率为450 W,反应时间为12 min时,其COD、腐殖质和色度的去除率达到了70.06%、94.61%和98.86%.与此同时,控制实验表明MW/Fe-C/H_2O_2具有较强的协同作用,且对有机物的降解效果远好于其他体系.经过MW/Fe-C/H_2O_2体系处理后,浓缩液中溶解性有机物的芳香性程度和腐殖质缩合度逐渐降低,并且腐殖质等大分子难降解有机物大幅去除,可生化性(BOD/COD值)也大幅提升.一方面,Fe-C材料包含了多种铁基氧化物等活性物质可与H_2O_2形成非均相芬顿反应;另一方面,在酸性条件下铁缓释淋滤产生的铁离子会与H_2O_2形成芬顿反应.并且,微波辐射作用可一定程度上强化上述过程,从而加速了有机物的去除.因此,MW/Fe-C/H_2O_2体系能够快速高效的对渗滤液浓缩液进行预处理,研究为高浓度有机废水的处理提供了借鉴.
In this study, the Fe-C catalyzed H_2O_2 process enhanced by microwave radiation(MW/Fe-C/H_2O_2 process) was applied to the pre-treatment of refractory organics in landfill leachate membrane concentrates. The effects of H_2O_2 dosage, Fe-C dosage, initial pH, and microwave intensity on refractory organics removals were systematically investigated. In addition, the synergetic effect of MW/Fe-C/H_2O_2 process was investigated. Transformation of dissolved organic matter was explored by UV-Vis and 3 D-EEM analysis. Finally, the material(Fe-C) were characterized by SEM-EDS and XRD in order to explore the catalysis mechanism of MW/Fe-C/H_2O_2 process. Results show that the removal rates of COD, humic substances(indicated by absorbance at 254 nm), and color number(CN) were 70.06%, 94.61%, and 98.86%, respectively, under conditions of H_2O_2 dose=10 mL·L~(-1), Fe-C dose=0.8 g·L~(-1), initial pH=3, microwave power=450 W, and reaction time=12 min. Moreover, the MW/Fe-C/H_2O_2 process exhibited a significant synergetic effect, and the treatment efficacy of MW/Fe-C/H_2O_2 process was much better than that of any other processes performed in this study. After the treatment of MW/Fe-C/H_2O_2 process, the aromatics and humic substances in dissolved organic matter were gradually reduced in membrane concentrates. Meanwhile, the biodegradability(BOD/COD ratio) was improved significantly. According to SEM-EDS and XRD analysis results, the treatment efficacy of MW/Fe-C/H_2O_2 process can be attributed to several aspects: ① Fe-C material contained a variety of active matters, such as iron-based oxidants, that can react with H_2O_2 to form heterogeneous Fenton system; ②the acidic ambient accelerated iron leaching, therefore homogeneous Fenton system was formed by Fe~(2+) and H_2O_2; and ③microwave radiation promoted the reaction kinetics,thus enhanced the removal of organic pollutants. In conclusion, MW/Fe-C/H_2O_2 process was efficient in the pre-treatment of refractory organics in membrane concentrates from landfill leachate. This study aimed to provide a technical reference for the treatment of high organic wastewater.
In this study, the Fe-C catalyzed H_2O_2 process enhanced by microwave radiation(MW/Fe-C/H_2O_2 process) was applied to the pre-treatment of refractory organics in landfill leachate membrane concentrates. The effects of H_2O_2 dosage, Fe-C dosage, initial pH, and microwave intensity on refractory organics removals were systematically investigated. In addition, the synergetic effect of MW/Fe-C/H_2O_2 process was investigated. Transformation of dissolved organic matter was explored by UV-Vis and 3 D-EEM analysis. Finally, the material(Fe-C) were characterized by SEM-EDS and XRD in order to explore the catalysis mechanism of MW/Fe-C/H_2O_2 process. Results show that the removal rates of COD, humic substances(indicated by absorbance at 254 nm), and color number(CN) were 70.06%, 94.61%, and 98.86%, respectively, under conditions of H_2O_2 dose=10 mL·L~(-1), Fe-C dose=0.8 g·L~(-1), initial pH=3, microwave power=450 W, and reaction time=12 min. Moreover, the MW/Fe-C/H_2O_2 process exhibited a significant synergetic effect, and the treatment efficacy of MW/Fe-C/H_2O_2 process was much better than that of any other processes performed in this study. After the treatment of MW/Fe-C/H_2O_2 process, the aromatics and humic substances in dissolved organic matter were gradually reduced in membrane concentrates. Meanwhile, the biodegradability(BOD/COD ratio) was improved significantly. According to SEM-EDS and XRD analysis results, the treatment efficacy of MW/Fe-C/H_2O_2 process can be attributed to several aspects: ① Fe-C material contained a variety of active matters, such as iron-based oxidants, that can react with H_2O_2 to form heterogeneous Fenton system; ②the acidic ambient accelerated iron leaching, therefore homogeneous Fenton system was formed by Fe~(2+) and H_2O_2; and ③microwave radiation promoted the reaction kinetics,thus enhanced the removal of organic pollutants. In conclusion, MW/Fe-C/H_2O_2 process was efficient in the pre-treatment of refractory organics in membrane concentrates from landfill leachate. This study aimed to provide a technical reference for the treatment of high organic wastewater.
引文
Amor C,De Torres-Socías E,Peres J A,et al.2015.Mature landfill leachate treatment by coagulation/flocculation combined with Fenton and solar photo-Fenton processes[J].Journal of Hazardous Materials,286:261-268
Scandelai A P J,Cardozo Filho L,Martins D C C,et al.2018.Combined processes of ozonation and supercritical water oxidation for landfill leachate degradation[J].Waste Management,77:466-476
Artinger R,Buckau G,Geyer S,et al.2000.Characterization of groundwater humic substances:influence of sedimentary organic carbon[J].Applied Geochemistry,15(1):97-116
Chen W,Westerhoff P,Leenheer J A,et al.2003.Fluorescence excitation-emission matrix regional integration to quantify spectra for dissolved organic matter [J].Environmental Science&Technology,37(24):5701-5710
崔东宇,何小松,席北斗,等.2015.堆肥腐熟前后胡敏酸与富里酸的还原容量比较[J].中国环境科学,35(7):2087-2094
管锡珺,赵亚鹏,智雪娇,等.2016.垃圾填埋场反渗透浓缩液回喷至附近垃圾焚烧厂焚烧研究[J].环境工程,34(5):123-125
郝瑞霞,曹可心,赵钢,等.2006.用紫外光谱参数表征污水中溶解性有机污染物[J].北京工业大学学报,32(12):1062-1066
康娟,周雯,权维强,等.2015.微波强化零价铁-芬顿法降解罗丹明B的研究[J].环境科学与技术,38(12):205-209
Li J Y,Zhao L,Qin L L,et al.2016.Removal of refractory organics in nanofiltration concentrates of municipal solid waste leachate treatment plants by combined Fenton oxidative-coagulation with photo-Fenton processes[J].Chemosphere,146:442-449
Li S,Zhang G,Wang P,et al.2016.Microwave-enhanced Mn-Fenton process for the removal of BPA in water[J].Chemical Engineering Journal,294:371-379
李民,陈炜鸣,蒋国斌,等.2017.Fe-Ce/GAC催化臭氧降解高浓度腐殖酸废水[J].环境科学学报,37(9):3409-3418
李晓东,高建民,于永川,等.2018.耦合微波的芬顿试剂/活性炭低温催化氧化NO[J].哈尔滨工业大学学报,50(1):90-95
刘导明,张璐,王磊,等.2018.机械蒸发处理垃圾渗滤液的试验研究[J].工业安全与环保,44(4):89-91
秦雅鑫.2016.Fe(Ⅲ)/H2O2类Fenton体系中Fe(Ⅲ)/Fe(Ⅱ)循环调控及其降解除草剂甲草胺性能的研究[D].武汉:华中师范大学
Segura Y,Martínez F,Melero J A.2013.Effective pharmaceutical wastewater degradation by Fenton oxidation with zero-valent iron[J].Applied Catalysis B Environmental,136-137(8):64-69
Huang T,Zhang G,Zhang N,et al.2018.Pre-magnetization by weak magnetic field enhancing Fe 0 -Fenton process for wastewater treatment[J].Chemical Engineering Journal,346:120-126
Tao S,Cui J,Zhang C S.1990.Spectroscopic characteristics of aquatic humic substances in the UV and visible region [J].Acta Geogra Sin,45(4):484-489
Wei X,Wu H,He G,et al.2017.Efficient degradation of phenol using iron-montmorillonite as a Fenton catalyst:Importance of visible light irradiation and intermediates[J].Journal of Hazardous Materials,321:408-416
王东梅,刘丹,刘庆梅,等.2014.渗滤液反渗透浓缩液回灌出水水质变化规律的研究[J].环境科学,35(7):2822-2829
王东梅,刘丹,李智,等.2017.渗滤液反渗透浓缩液回灌系统中盐分的迁移转化规律[J].环境工程学报,11(2):927-932
杨梦兵,王中伟,沈明.2010.垃圾渗滤液生化出水的脱色研究[J].污染防治技术,23(1):22-25
Zhang H,Zhang J,Zhang C,et al.2009.Degradation of C.I.Acid Orange 7 by the advanced Fenton process in combination with ultrasonic irradiation[J].Ultrasonics Sonochemistry,16(3):325-30
中华人民共和国国家统计局.2017.中国统计年鉴[M].北京:中国统计出版社
张爱平,陈炜鸣,李启彬,等.2018.MW-Fe0/H2O2体系预处理垃圾渗滤液浓缩液有机物[J].中国环境科学,38(6):2144-2156
郑可,周少奇,杨梅梅.2012.臭氧降解高浓度腐殖酸动力学[J].环境科学,33(3):879-884
郑可,周少奇,叶秀雅,等.2012.臭氧氧化法处理反渗透浓缩垃圾渗滤液[J].环境工程学报,6(2):467-470
曾萍,刘诗月,张俊珂,等.2017.芬顿法深度处理生物处理排水中的四环素抗性基因[J].中国环境科学,37(9):3315-3323
张爱平,李民,陈炜鸣,等.2017.臭氧降解村镇垃圾中转站渗滤液中有机污染物的试验研究[J].环境科学学报,37(2):694-702
朱佳裔.2011.FeOOH/H2O2去除水中对氯硝基苯的研究[D].哈尔滨:哈尔滨工业大学
Scandelai A P J,Cardozo Filho L,Martins D C C,et al.2018.Combined processes of ozonation and supercritical water oxidation for landfill leachate degradation[J].Waste Management,77:466-476
Artinger R,Buckau G,Geyer S,et al.2000.Characterization of groundwater humic substances:influence of sedimentary organic carbon[J].Applied Geochemistry,15(1):97-116
Chen W,Westerhoff P,Leenheer J A,et al.2003.Fluorescence excitation-emission matrix regional integration to quantify spectra for dissolved organic matter [J].Environmental Science&Technology,37(24):5701-5710
崔东宇,何小松,席北斗,等.2015.堆肥腐熟前后胡敏酸与富里酸的还原容量比较[J].中国环境科学,35(7):2087-2094
管锡珺,赵亚鹏,智雪娇,等.2016.垃圾填埋场反渗透浓缩液回喷至附近垃圾焚烧厂焚烧研究[J].环境工程,34(5):123-125
郝瑞霞,曹可心,赵钢,等.2006.用紫外光谱参数表征污水中溶解性有机污染物[J].北京工业大学学报,32(12):1062-1066
康娟,周雯,权维强,等.2015.微波强化零价铁-芬顿法降解罗丹明B的研究[J].环境科学与技术,38(12):205-209
Li J Y,Zhao L,Qin L L,et al.2016.Removal of refractory organics in nanofiltration concentrates of municipal solid waste leachate treatment plants by combined Fenton oxidative-coagulation with photo-Fenton processes[J].Chemosphere,146:442-449
Li S,Zhang G,Wang P,et al.2016.Microwave-enhanced Mn-Fenton process for the removal of BPA in water[J].Chemical Engineering Journal,294:371-379
李民,陈炜鸣,蒋国斌,等.2017.Fe-Ce/GAC催化臭氧降解高浓度腐殖酸废水[J].环境科学学报,37(9):3409-3418
李晓东,高建民,于永川,等.2018.耦合微波的芬顿试剂/活性炭低温催化氧化NO[J].哈尔滨工业大学学报,50(1):90-95
刘导明,张璐,王磊,等.2018.机械蒸发处理垃圾渗滤液的试验研究[J].工业安全与环保,44(4):89-91
秦雅鑫.2016.Fe(Ⅲ)/H2O2类Fenton体系中Fe(Ⅲ)/Fe(Ⅱ)循环调控及其降解除草剂甲草胺性能的研究[D].武汉:华中师范大学
Segura Y,Martínez F,Melero J A.2013.Effective pharmaceutical wastewater degradation by Fenton oxidation with zero-valent iron[J].Applied Catalysis B Environmental,136-137(8):64-69
Huang T,Zhang G,Zhang N,et al.2018.Pre-magnetization by weak magnetic field enhancing Fe 0 -Fenton process for wastewater treatment[J].Chemical Engineering Journal,346:120-126
Tao S,Cui J,Zhang C S.1990.Spectroscopic characteristics of aquatic humic substances in the UV and visible region [J].Acta Geogra Sin,45(4):484-489
Wei X,Wu H,He G,et al.2017.Efficient degradation of phenol using iron-montmorillonite as a Fenton catalyst:Importance of visible light irradiation and intermediates[J].Journal of Hazardous Materials,321:408-416
王东梅,刘丹,刘庆梅,等.2014.渗滤液反渗透浓缩液回灌出水水质变化规律的研究[J].环境科学,35(7):2822-2829
王东梅,刘丹,李智,等.2017.渗滤液反渗透浓缩液回灌系统中盐分的迁移转化规律[J].环境工程学报,11(2):927-932
杨梦兵,王中伟,沈明.2010.垃圾渗滤液生化出水的脱色研究[J].污染防治技术,23(1):22-25
Zhang H,Zhang J,Zhang C,et al.2009.Degradation of C.I.Acid Orange 7 by the advanced Fenton process in combination with ultrasonic irradiation[J].Ultrasonics Sonochemistry,16(3):325-30
中华人民共和国国家统计局.2017.中国统计年鉴[M].北京:中国统计出版社
张爱平,陈炜鸣,李启彬,等.2018.MW-Fe0/H2O2体系预处理垃圾渗滤液浓缩液有机物[J].中国环境科学,38(6):2144-2156
郑可,周少奇,杨梅梅.2012.臭氧降解高浓度腐殖酸动力学[J].环境科学,33(3):879-884
郑可,周少奇,叶秀雅,等.2012.臭氧氧化法处理反渗透浓缩垃圾渗滤液[J].环境工程学报,6(2):467-470
曾萍,刘诗月,张俊珂,等.2017.芬顿法深度处理生物处理排水中的四环素抗性基因[J].中国环境科学,37(9):3315-3323
张爱平,李民,陈炜鸣,等.2017.臭氧降解村镇垃圾中转站渗滤液中有机污染物的试验研究[J].环境科学学报,37(2):694-702
朱佳裔.2011.FeOOH/H2O2去除水中对氯硝基苯的研究[D].哈尔滨:哈尔滨工业大学
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