紫外光芬顿-膜分离耦合体系降解金霉素

姚宏; 向鑫鑫; 薛宏慧; 孙绍斌; 张旭; 鲁垠涛; 张战胜

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中国环境科学 ›› 2020, Vol. 40 ›› Issue (4) : 1577-1585.

水污染与控制

紫外光芬顿-膜分离耦合体系降解金霉素

姚宏^1,2,3, 向鑫鑫^1,2,3, 薛宏慧^1,2,3, 孙绍斌^1,2,3, 张旭^1,2,3, 鲁垠涛^1,2,3, 张战胜⁴

作者信息 +

Study on degradation of chlortetracycline by photo-Fenton ceramic membrane coupling system

YAO Hong^1,2,3, XIANG Xin-xin^1,2,3, XUE Hong-hui^1,2,3, SUN Shao-bin^1,2,3, ZHANG Xu^1,2,3, LU Yin-tao^1,2,3, ZHANG Zhan-sheng⁴

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摘要

以金霉素为降解对象，采用沉淀法制备α-FeOOH光催化剂，进一步将其用共价结合法负载在陶瓷膜上，用SEM、XRD、EDS、UV-Vis和FTIR对α-FeOOH和光催化陶瓷膜进行表征.结果表明催化剂α-FeOOH呈针状或纺锤长片状，长宽分别为500~550nm、25~50nm，经α-FeOOH改性的陶瓷膜孔隙率由14.83%变为8.11%.研究光芬顿陶瓷膜耦合体系对金霉素的降解效率和动力学行为，确定了光芬顿陶瓷膜耦合体系的最优降解条件为金霉素初始浓度50mg/L，H₂O₂投加浓度10mmol/L，UV强度为3796.6μW/cm².进一步利用UV-Vis光谱分析了两种体系对金霉素的降解机理，光催化剂体系下，H₂O₂的浓度基本保持不变，而光芬顿陶瓷膜耦合体系下H₂O₂的浓度先升后降，同时后者在同一时间点对TOC和NH₄⁺-N去除率更高，表明光芬顿陶瓷膜耦合体系氧化能力更强，对金霉素的降解更为彻底.

Abstract

Rutheniummycin was used as the degradation target, and the α-FeOOH photocatalyst was prepared by precipitation method, and further loaded on the ceramic membrane by covalent bonding method and characterization of α-FeOOH and photocatalytic ceramic membranes by SEM, XRD, EDS, UV-Vis and FTIR. The results showed that the catalyst α-FeOOH was acicular or spindle-shaped, with a length and width of 500~550nm and 25~50nm, respectively. The porosity of the ceramic membrane modified by α-FeOOH is changed from 14.83% to 8.11%. The degradation efficiency and kinetic behavior of fentanyl ceramic membrane coupling system were studied. The optimal degradation conditions of the photo-Fenton ceramic membrane coupling system were determined as the initial concentration of chlortetracycline 50mg/L, H₂O₂ concentration 10mmol/L, UV intensity 3796.6μW/cm². The degradation mechanism of chlortetracycline in the two systems was further analyzed by UV-Vis spectroscopy. Under the photocatalyst system, the concentration of H₂O₂ remained basically unchanged, while the concentration of H₂O₂ in the photo-Fenton ceramic membrane coupling system first rose and then decreased, and the latter had higher removal rates of TOC and NH₄⁺-N at the same time point, indicating that the photo-Fenton ceramic membrane coupling system has stronger oxidizing ability and more complete degradation of chlortetracycline.

导出引用

姚宏, 向鑫鑫, 薛宏慧, 孙绍斌, 张旭, 鲁垠涛, 张战胜. 紫外光芬顿-膜分离耦合体系降解金霉素[J]. 中国环境科学. 2020, 40(4): 1577-1585

YAO Hong, XIANG Xin-xin, XUE Hong-hui, SUN Shao-bin, ZHANG Xu, LU Yin-tao, ZHANG Zhan-sheng. Study on degradation of chlortetracycline by photo-Fenton ceramic membrane coupling system[J]. China Environmental Science. 2020, 40(4): 1577-1585

中图分类号： X703.5

参考文献

[1] 李明亮.环境中磺胺类药物的降解行为及影响因素的研究[D]. 新乡:河南师范大学, 2012. Li M R. Study of the degradation of sulfonamides under various environment conditions and its influencing factors[D]. Xinxiang:Henan Normal University, 2012.
[2] Liu Y, Wang C, Sui Z, et al. Degradation of chlortetracycline using nano micro-electrolysis materials with loading copper[J]. Separation and Purification Technology, 2018,203:29-35.
[3] Patyra E, Kowalczyk E, Grelik A, et al. Screening method for the determination of tetracyclines and fluoroquinolones in animal drinking water by liquid chromatography with diode array detector[J]. Polish Journal of Veterinary Sciences, 2015,18(2):283-289.
[4] Wang N, Guo X, Xu J, et al. Pollution characteristics and environmental risk assessment of typical veterinary antibiotics in livestock farms in Southeastern China[J]. Journal of Environmental Science and Health, Part B, 2014,49(7):468-479.
[5] Antibiotics, antibiotic resistance genes, and bacterial community composition in fresh water aquaculture environment in China[J]. Microbial Ecology, 2015,70(2):425-432.
[6] 魏瑞成,葛峰,陈明,等.江苏省畜禽养殖场水环境中四环类抗生素污染研究[J]. 农业环境科学学报, 2010,29(6):1205-1210. Wei R C, Ge F, Chen M, et al. Pollution of tetracyclines from livestock and poultry farms in aquatic environment in Jiangsu Province, China[J]. Journal of Agro-Environment Science, 2010,29(6):1205-1210.
[7] Pulicharla R, Brar S K, Rouissi T, et al. Degradation of chlortetracycline in wastewater sludge by ultrasonication, Fenton oxidation, and ferro-sonication[J]. Ultrasonics Sonochemistry, 2017, 34:332-342.
[8] Liao X, Zou R, Li B, et al. Biodegradation of chlortetracycline by acclimated microbiota[J]. Process Safety and Environmental Protection, 2017,109:11-17.
[9] 张成武,李天一,廉静茹,等.Fe(II)活化O₂高级氧化降解罗丹明B染料[J]. 中国环境科学, 2018,38(2):560-565. Zhang C W, Li T Y, Lian J R, et al. Study on degradation of rhodamine B by advanced oxidation based on O₂ activation by Fe(Ⅱ)[J]. China Environmental Science, 2018,38(2):560-565.
[10] 陈珊珊.基于γ-Fe₂O₃膨润土光芬顿体系的构建及催化降解染料研究[D]. 石河子:石河子大学, 2012. Chen S S. Construction and catalytic degradation of dyes based on γ-Fe₂O₃ bentonite photo-Fenton system[D]. Shihezi:Shihezi University, 2012.
[11] 赵芙蓉,王飞,耿环环,等. g-C₃N₄/Ag/α-FeOOH对磺胺嘧啶的光催化降解效果评价[J]. 化学与生物工程, 2019,36(1):24-28. Zhao F R, Wang F, Geng H H, et al. Photocatalytic degradation of sulfadiazine using g-C₃N₄/Ag/α-FeOOH[J]. Chemistry & Bioengineering, 2019,36(1):24-28.
[12] Papi? S, Vujevi? D, Koprivanac N, et al. Decolourization and mineralization of commercial reactive dyes by using homogeneous and heterogeneous Fenton and UV/Fenton processes[J]. Journal of Hazardous Materials, 2009,164(2/3):1137-1145.
[13] 刘婷.非均相光芬顿体系的建立与内循环流化床反应器的研究[D]. 哈尔滨:哈尔滨工业大学, 2009. Liu T. Establishment of heterogeneous photo-Fenton systemand research on circulation fluidized-bed reactor[D]. Harbin:Harbin Institute of Technology, 2009.
[14] Li X, Wang J, Rykov A I, et al. Prussian blue/TiO₂ nanocomposites as a heterogeneous photo-Fenton catalyst for degradation of organic pollutants in water[J]. Catalysis Science & Technology, 2014,5(1):504-514.
[15] Zhao G, Huang Q, Rong X, et al. Biodegradation of methyl parathion in the presence of goethite:The effect of Pseudomonas sp. Z1adhesion[J]. International Biodeterioration & Biodegradation, 2014,86:294-299.
[16] 孙绍斌.陶瓷膜耦合光芬顿体系构建及其对磺胺类抗生素降解机制研究[D]. 北京:北京交通大学, 2019. Sun S B. Study on the degradation mechanism of the Sulfa antibiotics by by ceramic membrane coupling withphoto-Fenton system[D]. Beijing:Beijing Jiaotong University, 2019.
[17] Sun S B, Yao H, et al. Reactive photo-Fenton ceramic membranes:Synthesis, characterization and antifouling performance[J]. Water Research, 2018.
[18] Pulicharla R, Das R K, Brar S K, et al. Degradation kinetics of chlortetracycline in wastewater using Ultrasonication assisted laccase[J]. Chemical Engineering Journal, 2018,347:828-835.
[19] Yu-Hsiang W, Kuan-Chung C. Removal of disinfection by-products from contaminated water using a synthetic goethite catalyst via catalytic ozonation and a biofiltration system[J]. International Journal of Environmental Research and Public Health, 2014,11(9):9325-9344.
[20] Pouran H M, Banwart S A, Romero-Gonzalez M. Coating a polystyrene well-plate surface with synthetic hematite, goethite and aluminium hydroxide for cell mineral adhesion studies in a controlled environment[J]. Applied Geochemistry, 2014,42:60-68.
[21] Alhayek N, M Doré. Oxydation des phenols par le peroxyde d'hydrogene en milieu aqueux en presence de fer supporte sur alumine[J]. Water Research, 1990,24(8):973-982.
[22] Oliveira L C A, Ramalho T C, Eugênio F. Souza, et al. Catalytic properties of goethite prepared in the presence of Nb on oxidation reactions in water:Computational and experimental studies[J]. Applied Catalysis B Environmental, 2008,83(3/4):169-176.
[23] Neamtu M, Catrinescu C, Kettrup A. Effect of dealumination of iron(III)-exchanged Y zeolites on oxidation of Reactive Yellow 84azo dye in the presence of hydrogen peroxide[J]. Applied Catalysis B, 2004,51(3):149-157.
[24] Rong S P, Sun Y B, Zhao Z H. Degradation of sulfadiazine antibiotics by water falling film dielectric barrier discharge[J]. Chinese Chemical Letters, 2014,25(1):187-192.
[25] Baeza C, Knappe D R U. Transformation kinetics of biochemically active compounds in low-pressure UV photolysis and UV/H₂O₂ advanced oxidation processes[J]. Water Research, 2011,45(15):0-4543.