Cover Image

Adsorptive Removal Study of the Frequently Used Fluoroquinolone Antibiotics - Moxifloxacin and Norfloxacin from Wastewaters using Natural Zeolites

Imeda Rubashvili, Luba Eprikashvili, Teimuraz Kordzakhia, Marine Zautashvili, Nino Pirtskhalava, Maia Dzagania

Abstract


Residual antibiotics pollution has become one of the most severe environmental problems today.  Antibiotics from hospitals and drug factories represent a potential risk for human and ecological health. Therefore, it has been a high exigency to develop some efficient and cost-effective treatment methods and technologies for antibiotics removal from industrial and household contaminated water. Adsorption is one of the most utilised techniques and has many competitive advantages such as the unique properties of flexibility, effectiveness, superior performance and the robustness for consecutive cycles. The present research concerns the adsorption of two frequently used fluoroquinolone antibiotics - moxifloxacin and norfloxacin on natural zeolite - clinoptilolite and its acid-modified form from aqueous solutions. For the first time, the adsorption of the antibiotics mentioned above on the selected natural zeolite was investigated under static and dynamic conditions. Adsorption experiment under dynamic conditions carried out using the specially constructed dynamic type of laboratory equipment. The effect of the inlet concentration, the flow rate and the pH value of the antibiotic solution, also, the contact time of system zeolite/antibiotic solution on the adsorption process were examined and evaluated using the Langmuir and Freundlich adsorption models. The results showed that the highest static adsorption capacities were observed at low initial concentration - 0.2 mg/mL of antibiotic solution for both adsorbents; the highest dynamic adsorption capacities - at low flow rate - 1.5 mg/mL and low inlet concentration - 0.2 mg/mL of antibiotic solution for both adsorbents. The static adsorption capacity was up to 2.71 mg/g for moxifloxacin hydrochloride; 4.14 mg/g for norfloxacin and the dynamic adsorption capacity was up to 1.20 mg/g for moxifloxacin hydrochloride; 2.10 mg/g for norfloxacin at a neutral pH value and constant temperature of 200°C. Each antibiotic was determined quantitatively in sample solutions using the developed and validated HPLC methods with a limit of quantitation - 0.05 µg/mL. Hence, this study demonstrates and proves that natural zeolite could be an effective adsorbent for the removal of the selected antibiotics from wastewaters.


Full Text:

PDF

References


- A. Fleming, The discovery of penicillin, Br. Med. Bull, 1944, 2, 4-5.

- K. Kummerer, Antibiotics in the aquatic environment - A review - Part I, Chemosphere, 2009, 75(4), 417-434.

- R. Wise, Antimicrobial resistance: priorities for action, J. of Antimicrob. Chemother., 2002, 49(4), 585-586.

- S.T. Glassmeyer, E.K. Hinchey, S.E. Boehme, C.G. Daughton, I.S. Ruhoy, O. Conerly, R.L. Daniels, L. Lauer, M. McCarthy, T.G. Nettesheim, K. Sykes, and V.G. Thompson, Disposal practices for unwanted residential medications in the United States, Environ. Int., 2009, 35(3), 566-572.

- F.Yu, Y. Li, S. Han, J. Ma, Adsorptive removal of antibiotics from aqueous solution using carbon materials, Chemosphere, 2016, 153, 365-385.

- G. Moussavi, A. Alahabadi, K. Yaghmaeian, M. Eskandari, Preparation, characterization and adsorption potential of the NH4Cl-induced activated carbon for the removal of amoxicillin antibiotic from water, Chem. Eng. J., 2013, 217, 119-128.

- X. Chang, M.T. Meyer, X. Liu, Q. Zhao, H. Chen, J.-a. Chen, Z. Qiu, L. Yang, J. Cao, W. Shu, Determination of antibiotics in sewage from hospitals, nursery and slaughterhouse, wastewater treatment plant and source water in Chongqing region of Three Gorge Reservoir in China, Environ.l Pollut., 2010, 158(5), 1444-1450.

- K.D. Brown, J. Kulis, B. Thomson, T.H. Chapman, D.B. Mawhinney, Occurrence of antibiotics in the hospital, residential, and dairy effluent, municipal wastewater, and the Rio Grande in New Mexico, Sci. Total Environ., 2006, 366(2-3), 772-783.

- A.J. Watkinson, E.J. Murby, D.W. Kolpin, S.D. Costanzo, the occurrence of antibiotics in an urban watershed: From wastewater to drinking water. Sci. Total Environ., 2009, 407(8), 2711-2723.

- M. Hernando, M. Mezcua, A. Fernandezalba, D. Barcelo, Environmental risk assessment of pharmaceutical residues in wastewater effluents, surface waters and sediments, Talanta, 2006, 69(2), 334-342.

- S.D., Costanzo, J. Murby, J. Bates, Ecosystem response to antibiotics entering the aquatic environment, Mar. Pollut. Bull., 2005, 51(1-4), 218-223.

- J.J. Holstein, C.B. Hübschle, B. Dittrich, Electrostatic properties of ninefluoroquinolone antibiotics derived directly from their crystal structure refinements, Cryst. Eng. Comm., 2012, 14, 2520-2531.

- L.E. Bryan, J. Bedard, S. Wong, S. Chamberland, Quinolone antimicrobial agents: Mechanism of action and resistance development, Clin. Invest. Med., 1989, 12, 14-19.

- E.M. Golet, A.C. Alder, W. Giger, Environmental exposure and risk assessment of fluoroquinolone antibacterial agents in wastewater and river water of the Glatt Valley Watershed, Switzerland, Environ. Sci. Technol., 2002, 36, 3645-3651.

- B. Prutthiwanasan, C. Phechkrajang, L. Suntornsuk, Fluorescent labeling of ciprofloxacin and norfloxacin and its application for residues analysis in surface water, Talanta, 2016, 159, 74-79.

- Ai Jia, Yi Wan, Yang Xiao, Jianying Hu, Occurrence and fate of quinolone and fluoroquinolone antibiotics in a municipal sewage treatment plant, Water Res., 2012, 46(2), 387-394.

- T.A. Choi, Side Effects of Drugs Annual; Chapter 26 - Miscellaneous antibacterial drugs; Volume 35; Ed. by J.K. Aronson; Elsevier: Amsterdam, 2014, pp. 463-481.

- M.T. Darweesh, M.J. Ahmed, Adsorption of ciprofloxacin and norfloxacin from aqueous solution onto granular activated carbon in fixed-bed column, Ecotoxicol. Environ. Safety, 2017, 138 139-145.

- S. Suzuki, P.T. Phuong Hoa, Distribution of quinolones, sulfonamides, tetracyclines in an aquatic environment and antibiotic resistance in Indochina, Front. Microbio., 2012, 3(67).

- I.T. Carvalho, L. Santos, Antibiotics in the aquatic environments: A review of the European scenario, Environ. Int., 2016, 94, 736-757.

- US Pharmacopeia National Formulary USP 41-NF-36, Moxifloxacin, The United States Pharmacopeial Convention; United Book Press, Inc: Baltimore, 2018, pp. 8361-8363.

- US Pharmacopeia National Formulary USP 41-NF-36. Norfloxacin, The United States Pharmacopeial Convention; United Book Press, Inc: Baltimore, 2018, pp. 2976-2977.

- N. Le-Minh, S.J. Khan, J.E. Drewes, R.M. Stuetz, Fate of antibiotics during municipal water recycling treatment processes, Water Res., 2010, 44(15), 4295-4323.

- J. Torres-Pérez, C. Gérente, Y. Andrès, Sustainable activated carbons from agricultural residues dedicated to antibiotic removal by adsorption, Chin. J. Chem. Eng., 2012, 20, 524-529.

- L. Zhu, B. Santiago-Schübel, H. Xiao, H. Hollert, S. Kueppers, S., Electrochemical oxidation of fluoroquinolone antibiotics: mechanism, residual antibacterial activity and toxicity change, Water Res., 2016, 102, 52-62.

- M. Cˇvancˇarová, M. Moeder, A. Filipová, T. Cajthaml, Biotransformation of fluoroquinolone antibiotics by ligninolytic fungi-metabolites, enzymes and residual antibacterial activity, Chemosphere, 2015, 136, 311-320.

- F. Maraschi, M. Sturini, A. Speltini, L. Pretali, A. Profumo, A. Pastorello, TiO2-modified zeolites for fluoroquinolones removal from wastewaters and reuse after solar light regeneration, J. Environ. Chem. Eng., 2014, 2, 2170-2176.

- M. Feng, X. Wang, J. Chen, R. Qu, Y. Sui, L. Cizmas, Z. Wang, V.K. Sharma, Degradation of fluoroquinolone antibiotics by ferrate (VI): effects of water constituents and oxidized products. Water Res. 2016, 103, 48-57.

- B. Ebrahimpour, Y. Yamini, M. Moradi, Application of ionic surfactant as a carrier and emulsifier agent for the microextraction of Fluoroquinolones, J. Pharm. Biomed. Anal., 2012, 66, 264-270.

- H. Guo, N. Gao, Y. Yang, Y. Zhang, Kinetics and transformation pathways on oxidation of Fluoroquinolones with thermally activated persulfate, Chem. Eng. J., 2016, 292, 82-91.

- V.R.A. Ferreira, C.L. Amorim, S.M. Cravo, M.E. Tiritan, Fluoroquinolones biosorption onto microbial biomass: activated sludge and aerobic granular sludge, Int. Biodeterior. Biodegrad., 2016, 110, 53-60.

- F. Tan, D. Sun, J. Gao, Q. Zhao, X. Wang, F. Teng, X. Quan, J. Chen, Preparation of molecularly imprinted polymer nanoparticles for selective removal of fluoroquinolone antibiotics in aqueous solution, J. Hazard. Mater., 2013, 244–245, 750-757.

- I. Braschi, G. Gatti, G. Paul, C.E. Gessa, M. Cossi, L. Marchese, Sulfonamide antibiotics embedded in high silica zeolite Y: a combined experimental and theoretical study of host-guest and guest-guest interactions, Langmuir, 2010, 26(12), 9524-9532.

- J. Cao, C. Lei, B. Yang, Z. Li, L. Lei, Y. Hou, X. Feng, Zeolitic imidazolate framework derived core-shell-structured CoS2/CoS2-N-C supported on electrochemically exfoliated graphene foil for efficient oxygen evolution, Batt. Supercaps, 2018, 1, 1-8.

- A. Zukal, M. Shamzhy, M. Kubů, J. Čejka, The effect of pore size dimensions in isoreticular zeolites on carbon dioxide adsorption heats, J. CO2 Util., 2018, 24, 157-163.

- Z. Chen, W. Maa, G. Lub, F. Menga, S. Duana, Z. Zhanga, L. Weic, Y. Pana, Adsorption of levofloxacin onto mechanochemistry treated zeolite: Modeling and site energy distribution analysis, Sep. Purif. Technol., 2019, 222, 30-34.

- S.S. Salih, T.K. Ghosh, Preparation and characterization of chitosan-coated diatomaceous earth for hexavalent chromium removal, Environ. Processes, 2018, 5, 23-39.

- S.S. Salih, T.K. Ghosh, Preparation and characterization of bioadsorbent beads for chromium and zinc ions adsorption, Cogent Environ. Sci., 2017, 3, 1401577.

- S.S. Salih, T.K. Ghosh, Adsorption of Zn(II) ions by chitosan coated diatomaceous earth, Int. J. Biol. Macromol., 2018, 106, 602-610.

- Z. Liang, Z. Zhao, T. Sun, W. Shi, F. Cui, Adsorption of quinolone antibiotics in spherical mesoporous silica: effects of the retained template and its alkyl chain length, J. Hazard. Mater., 2016, 305, 8-14.

- H. Liu, W. Ning, P. Cheng, J. Zhang, Y. Wang, C. Zhang, Evaluation of animal hairs-based activated carbon for sorption of norfloxacin and acetaminophen by comparing with cattail fiber-based activated carbon, J. Anal. Appl. Pyrolysis, 2013, 101, 156-165.

- Y. Patiño, E. Díaz, S. Ordóñez, Pre-concentration of nalidixic acid through adsorption-desorption cycles: adsorbent selection and modeling, Chem. Eng. J., 2016, 283,486–494.

- A. Martucci, L. Pasti, N. Marchetti, A. Cavazzini, F. Dondi, A. Albertia, Adsorption of pharmaceuticals from aqueous solutions on synthetic zeolites, Micropor. Mesopor. Mater., 2012, 148(1), 174-183.

- D. Ašperger, I. Varga, S. Babić, L. Ćurković, Adsorption fenrofloxacine on natural zeolite – clinoptilolite, Holistic Approach Environ., 2014, 4(1), 3-15.

- G.V. Tsitsishvili, T.G. Andronikashvili, G.R. Kirov, and L.D. Filizova, Natural Zeolites; Ellis Horwood Limited: Chichester, 1991, p. 297.

- Y. Garci-Basabe, I. Rodriguez–Iznaga, L.C. De Menorval, P. Llewellyn, G. Maurin, D.W. Lewis, R. Binions, M. Autie, A.R. Ruiz-Salvador, Stepwise dealumination of natural clinoptilolite: Structural and physicochemical characterization, Micropor. Mesopor. Mater., 2010, 135, 187-196.

- Atlas of Zeolite Framework Types; ed by Ch. Baerlocher, L.B. McCucker, and D.H. Olson, Elsevier: Amsterdam, 2007, pp. 156-157.

- T.G. Andronikashvili, T.N. Kordzakhia, L.G. Eprikashvili, Zeolitese the Unique Desiccating Agents of Organic Liquids; Lap Lambert Academic Publishing, 2015, p.100.

- L.Eprikashvili, M.Zautashvili, T.Kordzakhia, N.Pirtskhalava, M.Dzagania, I. Rubashvili, V. Tsitsishvili, Intensification of bioproductivity of agricultural cultures by adding natural zeolites and brown coals into soils, Ann. Agr. Sci., 2016, 14, 67-71.

- I. Rubashvili, M. Zautashvili, T. Kordzakhia, L. Eprikashvili, Development and validation of quantitative determination HPLC methods of the fluoroquinolone antibiotics - moxifloxacin hydrochloride and norfloxacin in support of adsorption study on natural zeolites, Periódico Tchê Química, 2019, 16, 10-20 (Article in press).

- E. Milchert, W. Goc, R. Pelech, Adsorption of CCl4 from aqueous solution on activated carbons, Adsorpt. Sci. Technolog., 2000, 18, 823-837.

- D.N. Ribeiro de Sousa, S. Insa, A. A. Mozeto, M. Petrovic, T.F. Chaves, P.S. Fadini, Equilibrium and kinetic studies of the adsorption of antibiotics from aqueous solutions onto powdered zeolites, Chemosphere, 2018, 205, 137-146.

- M.M. Mohammed Ali, M.J. Ahmed, B.H. Hameed, NaY zeolite from wheat (Triticum aestivum L.) straw ash used for the adsorption of tetracycline, J. Clean. Prod., 2018, 172, 602-608.




DOI: http://dx.doi.org/10.13171/mjc92190921700ar

Refbacks

  • There are currently no refbacks.


Copyright (c) 2019 Mediterranean Journal of Chemistry