紫外/O3/过硫酸盐降解氯霉素的性能研究

常涛; 鲁仙; 吴文芳; 丁磊; 赵志淼; 张饮江

PDF(1380 KB)

中国环境科学 ›› 2025, Vol. 45 ›› Issue (5) : 2849-2856.

新污染物

紫外/O₃/过硫酸盐降解氯霉素的性能研究

常涛¹, 鲁仙^1,2, 吴文芳¹, 丁磊³, 赵志淼¹, 张饮江¹

作者信息 +

Performance study of chloramphenicol degradation by UV/O₃/peroxysulfate process

CHANG Tao¹, LU Xian^1,2, WU Wen-fang¹, DING Lei³, ZHAO Zhi-miao¹, ZHANG Yin-jiang¹

Author information +

文章历史 +

摘要

采用UV/O₃/PS工艺对氯霉素进行降解实验,研究了UV/O₃/PS联合工艺、UV/PS、O₃/PS及UV/O₃工艺对CAP的降解特性,分析了反应体系中主要活性自由基对氯霉素降解的贡献,分别考察了PS浓度、O₃浓度、pH值以及常见无机阴离子和天然有机物对降解的影响,探究了CAP的降解路径及消毒副产物的生成潜能,并计算了UV/O₃/PS工艺的能耗大小.结果表明,UV/O₃/PS联合工艺在60min时对氯霉素的去除率为90.41%;¹O₂、HO·和SO₄^·-为反应体系中3种主要的活性物种,其对氯霉素降解的贡献率依次为53.85%、25.64%和12.82%;PS和O₃浓度的增加有利于CAP的降解,碱性条件可促进CAP的降解,共存的Cl^-、HCO₃^-及腐殖酸对CAP降解存在抑制作用;氯霉素在UV/O₃/PS反应体系中降解机理主要包括羟基化、氨基氧化、C-N键断裂等步骤;CAP预氧化处理后其三氯甲烷和三氯乙腈的生成潜能显著增加,三氯甲烷生成潜能由30.35μg/L增加至48.08μg/L三氯乙腈生成潜能由12.31μg/L增长至20.97μg/L,能耗分析结果表明UV/O₃/PS工艺具有较好的综合效益.

Abstract

The UV/O₃/PS process was used for the degradation experiments of chloramphenicol, the degradation performance of the combined UV/O₃/PS process, UV/PS, O₃/PS and UV/O₃ processes was investigated, the contribution of major active free radicals to CAP degradation was analyzed for the reaction system, the effects of PS concentration, O₃ concentration, pH, and the common inorganic anions and natural organics on the degradation were examined respectively, the degradation pathway of CAP and the formation potential of disinfection by-products were clarified, also the calculation of energy consumption for the UV/O₃/PS process was discussed. The results showed that the CAP removal by the combined UV/O₃/PS process was 90.41% at 60min. ¹O₂, HO· and SO₄?^- were the three main active species in the reaction system, and their contributions to CAP degradation were 53.85%, 25.64% and 12.82% in turn. the ncrease of PS and O₃ concentrations favored the degradation of CAP, and alkaline conditions could promote the degradation of CAP, co-existing Cl^-, HCO₃^- and humic acid inhibited the degradation of CAP. the degradation mechanism of CAP by the UV/O₃/PS system mainly involved the hydroxylation, amino oxidation and C-N bond breaking or something. The formation potential of trichloromethane and trichloroacetonitrile was significantly increased through CAP pre-oxidation treatment, the formation potential for trichloromethane increased from 30.35μg/L to 48.08μg/L and that of trichloroacetonitrile from 12.31μg/L to 20.97μg/L. Energy consumption evaluation showed that the UV/O₃/PS process has a better overall efficiency.

导出引用

常涛, 鲁仙, 吴文芳, 丁磊, 赵志淼, 张饮江. 紫外/O₃/过硫酸盐降解氯霉素的性能研究[J]. 中国环境科学. 2025, 45(5): 2849-2856

CHANG Tao, LU Xian, WU Wen-fang, DING Lei, ZHAO Zhi-miao, ZHANG Yin-jiang. Performance study of chloramphenicol degradation by UV/O₃/peroxysulfate process[J]. China Environmental Science. 2025, 45(5): 2849-2856

中图分类号： X703

参考文献

[1] 闫霄珂.紫外活化亚硫酸盐降解水中氯霉素的机理研究[D].武汉:武汉理工大学, 2022. Yan X K. Mechanistic study on the degradation of chloramphenicol in water by UV-activated sulfite[D]. Wuhan: Wuhan University of Technology, 2022.
[2] 孙子为,高乃云,王奕岚.紫外激活过硫酸盐降解水中氯霉素的研究[J].中国给水排水, 2015,31(21):124-128. Sun Z W, Gao N Y, Wang Y L, et al.Study on UV-activated Persulfate Oxidation of Chloramphenicol in Water[J]. China Water& Wastewater, 2015,31(21):124-128.
[3] Deng W D, Zhang D Q, Zheng X X, et al. Removal of chloramphenicol by sulfide-modified nanoscale zero-valent iron activated persulfate: Performance, salt resistance, and reaction mechanisms[J]. Chemosphere, 2022,286:131876.
[4] W. G. Kramer, E. R. Rensimer, C. D. Ericsson, et al. Comparative bioavailability of intravenous and oral chloramphenicol in adults[J]. Journal of Clinical Pharmacology, 1984,24:181-186.
[5] Bu Q W, Wang B, Huang J, et al. Pharmaceuticals and personal care products in the aquatic environment in China: A review[J]. Journal of Hazardous Materials, 2013,262:189-211.
[6] Miklos D B, Wang W L, Linden K G, et al. Comparison of UV-AOPs (UV/H₂O₂, UV/PDS and UV/Chlorine) for TOrC removal from municipal wastewater effluent and optical surrogate model evaluation[J]. Chemical Engineering Journal, 2019,363:537-547.
[7] Zhong Y W, Shin K M, Diao Z H, et al. Peroxymonosulfate activation through LED-induced ZnFe₂O₄ for levofloxacin degradation[J]. Chemical Engineering Journal, 2021,417:129225.
[8] Liu B Z, Huang B R, Wang Z Z, et al. Homogeneous/heterogeneous metal-catalyzed persulfate oxidation technology for organic pollutants elimination: A review[J]. Journal of Environmental Chemical Engineering, 2023,11(3):109586.
[9] Dong G H, Chen B, Liu B, et al. Advanced oxidation processes in microreactors forwater and wastewater treatment: Development, challenges, and opportunities[J]. Water Research, 2022,211:118047.
[10] Jing L, Chen B, Zheng J S,et al. Ozonation of offshore produced water: kinetic study and fuzzy inference system modeling[J]. Environmental Monitoring and Assessment, 2018,190(11):132.
[11] Dong G H, Chen B, Liu B, et al. UV stimulated manganese dioxide for the persulfate catalytic degradation of bisphenol A[J]. Catalysts, 2021,11(4):502.
[12] Dong G H, Chen B, Liu B, et al. Comparison of O₃, UV/O₃, and UV/ O₃/PS processes for marine oily wastewater treatment: Degradation performance, toxicity evaluation, and flocs analysis[J]. Water Research, 2022,226:119234.
[13] Tan C Q, Fu D F, Gao N Y, et al. Kinetic degradation of chloramphenicol in water by UV/persulfate system[J]. Journal of Photochemistry and Photobiology A-chemistry, 2017,332:406-412.
[14] Lu X, Shao Y S, Gao N Y,et al. Investigation of clofibric acid removal by UV/persulfate and UV/chlorine processes: Kinetics and formation of disinfection byproducts during subsequent chlor (am) ination[J]. Chemical Engineering Journal, 2018,331:364-371.
[15] Zhang Y M, Chu W H, Xu T, et al. Impact of pre-oxidation using H₂O₂ and ultraviolet/H₂O₂ on disinfection byproducts generated from chlor (am) ination of chloramphenicol[J]. Chemical Engineering Journal, 2017,317:112-118.
[16] Yuan Z, Sui M H, Yuan B J, et al. Degradation of ibuprofen using ozone combined withperoxymonosulfate[J]. Environmental Sciencewater Research& Technology, 2017,3(5):960-969.
[17] Qin W L, Lin Z, Sun L, et al. A preliminary study on the integrated UV/ozone/persulfate Process for efficient abatement of atrazine[J]. Ozone-science& Engineering, 2020,42(6):558-564.
[18] Wang C, Zhao Z W, Deng X Y, et al. Ultrafast oxidation of emerging contaminants by novel VUV/Fe²⁺/PS process at wide pH range: Performance and mechanism[J]. Chemical Engineering Journal, 2021,426:131921.
[19] 相元泉.基于紫外光的高级氧化降解水中恩诺沙星机理研究[D].上海:上海海洋大学, 2022. Xiang Y Q. Study on the degradation mechanism ofenofloxacin from water with UV basedoxidation technology[D]. Shanghai: Shanghai ocean University, 2022.
[20] Yan Y Q, Wei Z S, Duan X G,et al. Merits and limitations of radical vs. nonradical pathways in persulfate-based advanced oxidation processes[J]. Environmental Science& Technology. 2023,57(33):12153-12179.
[21] Wang Y S, Song Y J, Li N, et al. Tunable active sites on biogas digestate derived biochar for sulfanilamide degradation by peroxymonosulfate activation[J]. Journal of Hazardous Materials, 2022,421:126794.
[22] 曾萍,刘诗月,张俊珂,等.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, 2017,37(9):3315-3323. Zeng P, Liu S Y, Zhang J K, et al. advanced Fenton oxidation treatment of tetracycline resistance genes in effluent discharged from biological wastewater treatment[J]. China Environmental Science, 2017,37(9): 3315-3323.
[23] Liu X H, Liu Y, Lu S Y, et al. Degradation difference of ofloxacin and levofloxacin by UV/H₂O₂ and UV/PS (persulfate): Efficiency, factors and mechanism[J]. Chemical Engineering Journal, 2020,385:123987.
[24] 孙鹏,张凯凯,张玉.向日葵秸秆生物炭强化Fe (Ⅲ)/S₂O₈^2--体系降解苯甲酸[J].环境科学, 2020,41(5):2301-2309. Zhang P, Zhang K K, Zhang Y, et al. Sunflower-straw-derived biochar-enhanced Fe (Ⅲ)/S₂O₈^2- system for degradation of benzoic acid[J]. Environmental Science, 2020,41(5):2301-2309.
[25] Wang Z Y, Shao Y S, Gao N Y, et al. Degradation kinetic of dibutyl phthalate (DBP) by sulfate radical- and hydroxyl radical-based advanced oxidation process in UV/persulfate system[J]. Separation and Purification Technology, 2018,195:92-100.
[26] Du J Y, Wang C, Sun M L, et al. Novel vacuum UV/ozone/ peroxymonosulfate process for efficient degradation of levofloxacin: Performance evaluation and mechanism insight[J]. Journal of Hazardous Materials, 2024,463:132916.
[27] Yu X B, Kamali M, Van Aken P,et al. Advanced oxidation of benzalkonium chloride in aqueous media under ozone and ozone/UV systems–Degradation kinetics and toxicity evaluation[J]. Chemical Engineering Journal, 2021,413:127431.
[28] Zhang B, Han Z W, Xin Y J,et al. Peroxymonosulfate activation by vacuum ultraviolet and trace copper ions: a new way to boost Cu (II)/Cu (I) redox cycle[J]. Chemical Engineering Journal, 2022,450: 138097.
[29] Byung-Taek O, Young-Suk S, Dega S,et al. Oxidative degradation of endotoxin by advanced oxidation process (O₃/H₂O₂& UV/H₂O₂)[J]. Journal of Hazardous Materials, 2014,279:105-110.
[30] Luo C W, Jiang J, Ma J, et al. Oxidation of the odorous compound 2,4,6-trichloroanisole by UV activated persulfate: Kinetics, products, and pathways[J]. Water Research, 2016,96:12-21.
[31] Li H C, Zhang X Y, Yang S, et al. Discerning the relevance of singlet oxygen in pollutant degradation in peroxymonosulfate activation processes[J]. Environmental Science& Technology, 2024,58(31): 14005-14012.
[32] 曹影.过一硫酸盐催化臭氧降解氯霉素效能及机理研究[D].哈尔滨:哈尔滨工业大学, 2018. Cao Y. Efficience and mechanism of chloramphenicol degradation byozone/peroxymonosulfate[D]. Haerbin: Harbin Institute of Technology, 2018.
[33] Xue J, Chen L, Wang H L, et al. Degradation mechanism of Alizarin Red in hybrid gas-liquid phase dielectric barrier discharge plasmas: Experimental and theoretical examination[J]. Chemical Engineering Journal, 2008,138:120-127.
[34] Zhang Y S, Shao Y S, Gao N Y, et al. Kinetics and by-products formation of chloramphenicol (CAP) using chlorination and photocatalytic oxidation[J]. Chemical Engineering Journal, 2018,333: 85-91.
[35] Chu W H, Chu T F, Bond T, et al. Impact of persulfate and ultraviolet light activated persulfate pre-oxidation on the formation of trihalomethanes, haloacetonitriles and halonitromethanes from the chlor (am) ination of three antibiotic chloramphenicols[J]. Water Research, 2016,93:48-55.
[36] Xie P C, Ma J, Liu W,et al. Impact of UV/persulfate pretreatment on the formation of disinfection byproducts during subsequent chlorination of natural organic matter[J]. Chemical Engineering Journal, 2015,269:203-211.
[37] Chu W H, Chu T F, Du E D, et al. Increased formation of halomethanes during chlorination of chloramphenicol in drinking water by UV irradiation, persulfate oxidation, and combined UV/ persulfate pre-treatments[J]. Ecotoxicology and Environmental Safety, 2016,124:147-154.
[38] Yu X P, Qin W L, Yuan X J, et al. Synergistic mechanism and degradation kinetics for atenolol elimination via integrated UV/ozone/ peroxymonosulfate process[J]. Journal of Hazardous Materials, 2021, 407:9.
[39] Sun P Z, Tyree C, Huang C H. Inactivation of Escherichia coli, bacteriophage MS2, and Bacillus spores under UV/H₂O₂ and UV/peroxydisulfate advanced disinfection conditions[J]. Environmental Science& Technology, 2016,50(8):4448-4458.