超声-Fenton试剂氧化耦合处理染料废水的研究
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摘要
偶氮染料废水由于其高色度、强毒性、难降解，在还原条件下易分解产生致癌性芳香胺，而被视为现今急待治理的废水之一。为此，本论文以偶氮染料活性艳红X-3B模拟废水为处理对象，采用超声波(US)-Fenton试剂联合的方法，以染料废水的降解率和紫外光谱所反映的结构变化进行降解效果的评价，较系统地研究了工艺条件对处理效果的影响，初步探讨了活性艳红X-3B的降解机制，并利用BOD_5／COD_(cr)比值法评价了染料废水的可生化性。
实验结果表明：活性艳红X-3B仅用超声处理，降解率为5％左右，仅用Fenton试剂处理，降解率为45％左右，而两者联合处理时，降解率可达90％以上，US-Fenton试剂耦合法明显优于二者的简单叠加，能够显著地缩短反应时间，提高降解率，是一种有效的处理染料废水的方法。并且US-Fenton法降解活性艳红X-3B符合二级反应动力学方程。
实验同时探讨了超声功率、变幅杆直径，溶液初始pH值、溶液温度以及FeSO_4和H_2O_2浓度等因素对活性艳红X-3B降解的影响。结果表明，温度对降解率的影响很小，可以忽略不计；而降解率会随超声功率的升高而升高；随溶液初始pH值升高而大幅度下降；随变幅杆直径增大呈现出先增加后减少的趋势；对于FeSO_4和H_2O_2则都存在一个最佳投加量。此外，对H_2O_2投加浓度、FeSO_4浓度、超声功率和溶液初始pH值等影响US-Fenton氧化过程的主要因素进行了正交实验分析，确定了各因素影响程度大小关系和最佳处理条件。
最后，文章利用BOD_5／COD_(cr)比值法评价染料的可生化性。结果表明，US-Fenton法处理后染料的可生化性有很大的提高。
Azo dyes wastewater is not only high chromatic, strong noxious, butalso difficult to degrade and easy to discompose to carcinogenic aromaticamine under deoxidization condition. So, azo dyes wastewater must betreated urgently. In this thesis, reactive-red X-3B solution, which has azodyes structure, was studied by Ultrasound-Fenton reagent techniques. Withthe degradation of reactive-red X-3B and the change of structure reflectedby UV spectrum as criteria, the influence of the technical conditions on thedisposal of reactive-red X-3B were systemically studied. Furthermore,decomposition mechanism of the azo dyes was studied and the ratio ofBiochemical Oxygen Demand to Chemical Oxygen Demand was used forthe dye's biodegradability study.
Degradation of simulated reactive-red X-3B wastewater by ultrasonictechnology, Fenton reagent oxidation, and a combination of the twoprocesses was studied. It was found that the degradation by ultrasonictechnology or Fenton reagent oxidation alone was insignificant, with adegradation rate-of 5% and 45% respectively; while it was greatly improvedwhen the two processes were combined, with a degra.dation rate up to 90%,which showed that these two processes presented a good synergetic effect.The degradation of reactive-red X-3B by the combined two processes couldbe described by second-order kinetics model.
The effect of many factors such as ultrasonic power, probe diameter, pH, temperature, concentration of FeSO_4 and H_2O_2 on the degradation ofreactive-red X-3B was investigated. The results showed that thetemperature had little or even an adverse effect on the degradation. Thedegradation rate was strongly pH dependent and increased with decreasingpH. On the contrary, the degradation rate was increased with increasingultrasonic power and FeSO_4 concentration, but it was increased slightlywhen FeSO_4 concentration was more than 0.045mmol/L, however, therewas an optimal H_2O_2 concentration for effective RR2 degradation.Furthermore, the orthogonal analyses were conducted to investigate suchsensitive effect factors as H_2O_2 concentration, FeSO_4 concentration,ultrasonic power and pH, and the optimum applicable parameters weredetermined.
Finally, the ratio of Biochemical Oxygen Demand to Chemical OxygenDemand is used for the dye's biodegradability study. The result showed thatthe dye's biodegradability has been heightened after ultrasonic technologyand Fenton reagent acting on it.
实验结果表明：活性艳红X-3B仅用超声处理，降解率为5％左右，仅用Fenton试剂处理，降解率为45％左右，而两者联合处理时，降解率可达90％以上，US-Fenton试剂耦合法明显优于二者的简单叠加，能够显著地缩短反应时间，提高降解率，是一种有效的处理染料废水的方法。并且US-Fenton法降解活性艳红X-3B符合二级反应动力学方程。
实验同时探讨了超声功率、变幅杆直径，溶液初始pH值、溶液温度以及FeSO_4和H_2O_2浓度等因素对活性艳红X-3B降解的影响。结果表明，温度对降解率的影响很小，可以忽略不计；而降解率会随超声功率的升高而升高；随溶液初始pH值升高而大幅度下降；随变幅杆直径增大呈现出先增加后减少的趋势；对于FeSO_4和H_2O_2则都存在一个最佳投加量。此外，对H_2O_2投加浓度、FeSO_4浓度、超声功率和溶液初始pH值等影响US-Fenton氧化过程的主要因素进行了正交实验分析，确定了各因素影响程度大小关系和最佳处理条件。
最后，文章利用BOD_5／COD_(cr)比值法评价染料的可生化性。结果表明，US-Fenton法处理后染料的可生化性有很大的提高。
Azo dyes wastewater is not only high chromatic, strong noxious, butalso difficult to degrade and easy to discompose to carcinogenic aromaticamine under deoxidization condition. So, azo dyes wastewater must betreated urgently. In this thesis, reactive-red X-3B solution, which has azodyes structure, was studied by Ultrasound-Fenton reagent techniques. Withthe degradation of reactive-red X-3B and the change of structure reflectedby UV spectrum as criteria, the influence of the technical conditions on thedisposal of reactive-red X-3B were systemically studied. Furthermore,decomposition mechanism of the azo dyes was studied and the ratio ofBiochemical Oxygen Demand to Chemical Oxygen Demand was used forthe dye's biodegradability study.
Degradation of simulated reactive-red X-3B wastewater by ultrasonictechnology, Fenton reagent oxidation, and a combination of the twoprocesses was studied. It was found that the degradation by ultrasonictechnology or Fenton reagent oxidation alone was insignificant, with adegradation rate-of 5% and 45% respectively; while it was greatly improvedwhen the two processes were combined, with a degra.dation rate up to 90%,which showed that these two processes presented a good synergetic effect.The degradation of reactive-red X-3B by the combined two processes couldbe described by second-order kinetics model.
The effect of many factors such as ultrasonic power, probe diameter, pH, temperature, concentration of FeSO_4 and H_2O_2 on the degradation ofreactive-red X-3B was investigated. The results showed that thetemperature had little or even an adverse effect on the degradation. Thedegradation rate was strongly pH dependent and increased with decreasingpH. On the contrary, the degradation rate was increased with increasingultrasonic power and FeSO_4 concentration, but it was increased slightlywhen FeSO_4 concentration was more than 0.045mmol/L, however, therewas an optimal H_2O_2 concentration for effective RR2 degradation.Furthermore, the orthogonal analyses were conducted to investigate suchsensitive effect factors as H_2O_2 concentration, FeSO_4 concentration,ultrasonic power and pH, and the optimum applicable parameters weredetermined.
Finally, the ratio of Biochemical Oxygen Demand to Chemical OxygenDemand is used for the dye's biodegradability study. The result showed thatthe dye's biodegradability has been heightened after ultrasonic technologyand Fenton reagent acting on it.
引文
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[2] 陈伟，范瑾初．超声降解水体中有机污染物技术综述[J]．上海环境科学，1999，18(10)：457-460
[3] Harkal U D,Gogate P R,Pandit A B. Ultrasonic degradation of poly (vinyl alcohol) in aqueous solution[J]. Ultrasonics Sonochemistry,2006,13(5):423-428
[4] 蹇锐．超声波降解水中有机污染物的研究进展[J]．湖南城市学院学报，2003，24(6)：105-108
[5] Stavarache C,Yim B,Vinatoru M,et al. Sonolysis of chlorobenzene in Fenton-type aqueous systems [J]. Ultrasonics Sonochemistry,2002,6(9):291-296
[6] Voncina D B,Marechal A. Reactive dye decolorization using combined ultrasound/H_2O_2[J]. Dyes and Pigments,2003,59(2):173-179
[7] 刘石生，丘泰球．超声在废水处理中的应用[J]．应用声学，2001，20(2)：43-46
[8] Hoffmann M R,Hua I,Hochemer R. Application of ultrasonic irradiation for the degradation of chemical contaminants in water[J]. Ultrasonics Sonochemistry,1996,3(3):163-172
[9] Bongbeen Y, Hiroshi O,Yoshio N,et al. Sonochemical degradation of chlorinated hydrocarbons using a batch and continuous flow system[J]. Journal of Hazardous Materials, 2001,81(3):253-263
[10] Jiang Y, Petrier C,Waite T D. Kinetics and mechanisms of ultrasonic degradation of volatile chlorinated aromatics in aqueous solutions[J]. Ultrasonics Sonochemistry,2002,9(6):317-323
[11] Gogate, Parag R. Cavitation:an auxiliary technique in wastewater treatment schemes[J]. Advances in Environmental Research,2002,3(6):335-358
[12] Nam S N,Han S K, Kang J W, et al. Kinetics and mechanisms of the sonolytic destruction of non-volatile organic compounds:investigation of the sonochemical reaction zone using several·OH monitoring techniques[J]. Ultrasonics Sonochemistry,2003,10(3):139-147
[13] Elefteria P, Grammatiki G, NicolaS K. Degradation of polycyclic aromatic hydrocarbons in aqueous solutions by ultrasonic irradiation[J]. Journal of Hazardous Materials,2004,108(1-2):95-102
[14] Yasui K, Tuziuti T, Iida Y. Optimum bubble temperature for the sonochemical production of oxidants[J]. Ultrasonics,2004,42(1-9):579-584
[15] Wang X,Yao Z,Wang J,et al. Degeadation of reactive brilliant red in aqueous solution by ultrasonic cavitation[J]. Ultrasonics Sonochemistry,2007,14(1):46-54
[16] Okitsu K, Iwasaki K, Yobiko Y, et al. Sonochemical degradation of azo dyes in aqueous solution:a new heterogeneous kinetics model taking into account the local concentration of OH radicals and azo dyes[J]. Ultrasonics Sonochemistry,2005,12(4):255-262
[17] Jiang Y, Petrier C,Waite T D. Effect of pH on the ultrasonic degradation of ionic aromatic compounds in aqueous solution[J]. Ultrasonics Sonochemistry,2002,9(3):163-168
[18] 马俊华，赵建夫，伊学农．超声技术在水处理上的研究进展[J]．上海环境科学，2002，21(5)：298-301
[19] Appaw C,Adewuyi Y G. Destruction of carbon disulfide in aqueous solutions by sonochemical oxidation[J]. Journal of Hazardous Materials,2002,90(3):237-249
[20] Inoue M,Okada F, Sakurai M,et al. A new development of dysstuffs degradation system using ultrasound[J]. Ultrasonics Sonochemistry,2006,13(4):313-320
[21] Vassilakis C,Pantidou A,Psillakis E,et al. Sonolysis of natural phenolic compounds in aqueous solutions:degradation pathways and biodegradation[J]. Water research,2004,38(13):3110-3118
[22] 陆永生，沈虹，华彬．含单环芳香烃废水的超卢降解实验研究[J]．上海环境科学，1999，18(11)：494-496
[23] Tezcanli-guyer G,Ince N H. Degradation and toxicity reduction of textile dyestuff by ultrasound[J]. Ultrasonics Sonochemistry,2003,10(4-5):235-240
[24] Godate P R,Pandit A B. Sonochemical reactors:scale up aspects[J]. Ultrasonics Sonochemistry, 2004,11(3-4): 105-117
[25] Sun J H,Sun S P, Sun J Y, et al. Degradation of azo dye Acid black i using low concentration iron of Fenton process facilitated by ultrasonic irradiation[J]. Ultrasonics Sonochemistry,2007,14(3):305-313
[26] Entezari M H,Heshmati A, Sarafraz-vazdi A. A combination of ultrasound and inorganic catalyst:removal of 2-chlorophenol from aqueous solution[J]. Ultrasonics Sonochemistry,2005,12(1-2):137-141
[27] Gogate P R,Mujumdar S,Pandit A B. Sonochemical reactors for waste water treatment: comparison using formic acid degradation as a model reaction[J]. Advances in Environmental Research,2003, 7(2):283-299
[28] Giancarlo C,Gabriele O,Livio S. An improved sonochemical reactor[J]. Ultrasonics Sonochemistry, 2005,12(3 ):213-217
[29] Svitelska, G V, Gallios, G P, Zouboulis, A I. Sonochemical decomposition of natural polyphenolic compound[J]. Chemosphere,2004,56(10):981-987
[30] 刘红，何韵华，欧阳威，等．超声波强化污水生物处理的可行性探讨[J]．重庆环境科学，2003，25(3)：18-20
[31] Eleni M,Elefleria P,Nicolas K, et al. Degradation of sodium dodecylbenzene sulfolfonate in water by ultrasonic irradiation[J]. Water Research,2004,38(17):3751-3759
[32] 李丹阳，陈刚，张光明．超声波预处理污泥研究进展[J]．环境污染治理技术与设备，2003，4(8)：70-72
[33] 陆少锋，李景川，王雪燕．Fenton试剂在印染中的应用前景[J]．印染，2003，(10)：41-45
[34] Palanivelu K, Kavitha V. Destruction of cresols by Fenton oxidation process[J]. Water Research,2005,39(13):3062-3072
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