DEGRADATION BEHAVIOR AND BIOLOGICAL RESPONSE OF CIPROFLOXACIN WASTEWATER BY INTIMATELY COUPLED PHOTOCATALYSIS AND BIODEGRADATION
-
摘要: 考察了光催化-生物降解直接耦合体系(ICPB)对环丙沙星(CIP)的降解行为,着重探讨了不同反应条件对ICPB体系降解CIP效率的影响及ICPB中生物响应与关键作用。结果表明:ICPB反应体系中,载体投加量为30%,光照强度为50 klux,反应初始pH值为7,ρ(DO)为5~6 mg/L时,CIP去除效果最佳,并可在较宽CIP浓度范围内(5~30 mg/L)具有较高的去除率,且其降解效率(90%)明显优于单独光催化(80%)和单独生物降解(50%)。生物膜观察结果阐明,ICPB载体内部生物膜未受到显著伤害,并且微生物通过利用CIP光催化氧化形成的小分子中间产物存活并对这些产物进行进一步生物降解,从而达到完全矿化。ICPB中生物膜通过Ferruginibacter、Clostridium、Stenotrophomonas和Comamonas等菌属的富集来适应环境胁迫,同时生物群落结构的演替对于微生物存活有着重要意义。
-
关键词:
- 光催化-生物法直接耦合 /
- 环丙沙星废水 /
- 降解行为 /
- 降解途径 /
- 生物响应
Abstract: The degradation behavior of ciprofloxacin (CIP) by intimately coupled photocatalysis and biodegradation system (ICPB) was investigated in this study. The effects of different reaction conditions on the degradation efficiency of CIP by ICPB system and the response and key role of organisms in ICPB were discussed. The results showed that the best CIP removal effect was achieved in the ICPB reaction system with a carrier dosage of 30%, a light intensity of 50 klux, an initial pH of 7 and a dissolved oxygen concentration of 5 to 6 mg/L, and a high removal efficiency could be kept in a wide range of initial CIP concentrations (5 to 30 mg/L), and the degradation efficiency (90%) was significantly better than that of photocatalysis alone (80%) and biodegradation alone (50%). The biofilm observation result clarified that biofilms inside the carriers of ICPB were not significantly damaged, and microorganisms survived by using the small molecule intermediates formed by the photocatalytic oxidation of CIP and, further biodegraded these products to achieve complete mineralization. The biofilms in ICPB adapt to environmental stress through the enrichment of Ferruginibacter, Clostridium, Stenotrophomonas and Comamonas, and the succession of the community structure was of great importance for the survival of microorganisms. -
[1] ZHANG Y J, BOYD S A, TEPPEN B J, et al. Organic acids enhance bioavailability of tetracycline in water to Escherichia coli for uptake and expression of antibiotic resistance[J]. Water Research, 2014, 65: 98-106. [2] OBEROI A S, JIA Y Y, ZHANG H Q, et al. Insights into the fate and removal of antibiotics in engineered biological treatment systems: a critical review[J]. Environmental Science & Technology, American Chemical Society, 2019, 53 (13): 7234-7264. [3] ZHANG Q Q, YING G G, PAN C G, et al. Comprehensive evaluation of antibiotics emission and fate in the river basins of China: source analysis, multimedia modeling, and linkage to bacterial resistance[J]. Environmental Science & Technology, American Chemical Society, 2015, 49 (11): 6772-6782. [4] MOVASAGHI Z, YAN B, NIU C. Adsorption of ciprofloxacin from water by pretreated oat hulls: equilibrium, kinetic, and thermodynamic studies[J]. Industrial Crops and Products, 2019, 127: 237-250. [5] JOHNSON A C, KELLER V, DUMONT E, et al. Assessing the concentrations and risks of toxicity from the antibiotics ciprofloxacin, sulfamethoxazole, trimethoprim and erythromycin in European rivers[J]. Science of the Total Environment, 2015, 511: 747-755. [6] SENTA I, TERZIC S, AHEL M. Occurrence and fate of dissolved and particulate antimicrobials in municipal wastewater treatment[J]. Water Research, 2013, 47 (2): 705-714. [7] JANECKO N, POKLUDOVA L, BLAHOVA J, et al. Implications of fluoroquinolone contamination for the aquatic environment-a review[J]. Environmental Toxicology and Chemistry, 2016, 35 (11): 2647-2656. [8] JIA Y Y, KHANAL S K, SHU H Y, et al. Ciprofloxacin degradation in anaerobic sulfate-reducing bacteria (SRB) sludge system: mechanism and pathways[J]. Water Research, 2018, 136: 64-74. [9] LI G Z, PARK S, KANG D W, et al. 2,4,5-Trichlorophenol degradation using a novel TiO2-coated biofilm carrier: roles of adsorption, photocatalysis, and biodegradation[J]. Environmental Science & Technology, American Chemical Society, 2011, 45 (19): 8359-8367. [10] LI G Z, PARK S, RITTMANN B E. Developing an efficient TiO2-coated biofilm carrier for intimate coupling of photocatalysis and biodegradation[J]. Water Research, 2012, 46 (19): 6489-6496. [11] MARSOLEK M D, TORRES C I, HAUSNER M, et al. Intimate coupling of photocatalysis and biodegradation in a photocatalytic circulating-bed biofilm reactor[J]. Biotechnology and Bioengineering, 2008, 101 (1): 83-92. [12] DONG Y L, XU D Y, WANG Q W, et al. Tailoring the electronic structure of ultrathin 2D Bi3O4Cl sheets by boron doping for enhanced visible light environmental remediation[J]. Applied Surface Science, 2021, 542: 148521. [13] 肖伽励, 周龙生, 王元有,等. Mg-Al LDH的制备及Mg-Al LDH/H2O2体系降解水中环丙沙星的研究[J]. 化学研究与应用, 2021, 33(4): 755-760. [14] 郭雲. 光催化与生物降解近场耦合协同作用强化方法与机制[D]. 长春:吉林大学, 2020. [15] 刘晓伟, 谢丹平, 李开明, 等. 溶解氧变化对底泥酶活性及微生物多样性的影响[J]. 环境科学与技术, 2013, 36(6): 6-11. [16] FROMM H J. The effect of temperature and ph on enzyme activity[G]. Initial Rate Enzyme Kinetics. Berlin, Heidelberg: Springer, 1975: 201-235. [17] 王旭,陈熙,徐新阳,等.CQDs/TiO2复合材料的制备及光催化降解抗生素[J].环境化学,2022,41(12):3876-3885. [18] 段飞阳, 周安宁, 陈福欣, 等. 石墨相氮化碳纳米片的可控制备及光催化性能[J]. 硅酸盐学报, 2021, 49(1): 2053-2060. [19] ZHANG X X, LI R P, JIA M K, et al. Degradation of ciprofloxacin in aqueous bismuth oxybromide (BiOBr) suspensions under visible light irradiation: a direct hole oxidation pathway[J]. Chemical Engineering Journal, 2015, 274: 290-297. [20] 熊厚锋. 可见光催化氧化—生物降解直接耦合技术降解四环素废水的效能与作用机制[D]. 长春:吉林大学, 2017. [21] XIE Z J, FENG Y P, WANG F L, et al. Construction of carbon dots modified MoO3/g-C3N4 Z-scheme photocatalyst with enhanced visible light photocatalytic activity for the degradation of tetracycline[J]. Applied Catalysis B: Environmental, 2018, 229: 96-104. [22] ZHANG B, JI M, QIU Z G, et al. Microbial population dynamics during sludge granulation in an anaerobic-aerobic biological phosphorus removal system[J]. Bioresource Technology, 2011, 102 (3): 2474-2480. [23] LIU Y Q, KONG Y H, ZHANG R, et al. Microbial population dynamics of granular aerobic sequencing batch reactors during start-up and steady state periods[J]. Water Science and Technology, 2010, 62 (6): 1281-1287. [24] SOLTAN MOHAMMADI N, MAFAKHERI S, ABDALI N, et al. Identification and characterization of the channel-forming protein in the cell wall of Corynebacterium amycolatum[J]. BBA-Biomembranes, 2013, 1828 (11): 2574-2582. [25] WALSH F, DUFFY B. The culturable soil antibiotic resistome: a community of Multi-Drug resistant bacteria[J]. PLoS ONE, 2013, 8 (6): e65567. [26] OLIVARES J, BERNARDINI A, GARCIA-LEON G, et al. The intrinsic resistome of bacterial pathogens[J]. Frontiers in Microbiology, 2013, 4: 103-112. [27] WOJCIESZYŃSKA D, GUZIK U, GREŃ I, et al. Induction of aromatic ring: cleavage dioxygenases in Stenotrophomonas maltophilia strain KB2 in cometabolic systems[J]. World J Microbiol Biotechnol, 2011, 27 (4): 805-811. [28] HUANG Z, NI B, JIANG C Y, et al. Direct sensing and signal transduction during bacterial chemotaxis toward aromatic compounds in Comamonas testosteroni[J]. Mol Microbiol, 2016, 101 (2): 224-237.
点击查看大图
计量
- 文章访问数: 330
- HTML全文浏览量: 21
- PDF下载量: 34
- 被引次数: 0