Evaluation of the Removal Efficiency of Diclofenac in the Aquatic Environment by Combined Coagulation and Adsorption Processes

Abstract

In decades, the presence of anti-inflammatory drugs diclofenac (DCF) in water resources has become an extremely threatening factor in terms of environmental protection and pollution. In this study, the removal efficiencies of DCF in aqueous sources were studied by adsorption, conventional coagulation, and combined coagulation methods using carbon nanotubes (CNTs). Experimental studies were carried out by adding certain doses of 1 g/L stock DCF solution prepared in the laboratory to water samples. In order to determine the adsorbing capacity of DCF, three different adsorbents as single-walled CNT (SWCNT), multi-walled CNT (MWCNT), and powdered activated carbon (PAC) were used as a function of pH and ionic strength. As a result of batch adsorption experiments performed in both ULW and UDWTP samples, the highest DCF sorption capacity was observed in SWCNT at pH =3 as 4.82 mg.g-1 and 3.82 mg.g-1, respectively, and also DCF adsorption capacity increased when the ionic strength was increased from 6.0×10-1 to 1.0 M. Furthermore, the experimental results showed that the Freundlich equation about correlation coefficient (R2=0.99) is the best isotherm model to describe the adsorption process in all water sources. On the other hand, results in coagulation experiments demonstrated that the maximum removal percentages of DCF in ULW (94.81%) and UDWTP (91.97%) occurred with combined SWCNT with Alum compared to only Alum coagulation. Experimental data obtained in this study reveal that combined coagulation with CNTs is more appropriate to minimize the pollution caused by DCF, especially in the aquatic environment, rather than adsorption and coagulation processes.

Keywords

• Diclofenac
• environmental protection
• adsorption
• combined coagulation

Supporting Institution

Zonguldak Bülent Ecevit University, Scientific Research Projects Commission

Project Number

2021-77047330-02

Thanks

The authors are indebted to the Zonguldak Bülent Ecevit University, Scientific Research Projects Commission (Project Number: 2021-77047330-02).

References

1. 1. Jain SN, Tamboli SR, Sutar DS, Jadhav SR. Marathe JV, Shaikh AA, Prajapati AA. Batch and continuous studies for adsorption of anionic dye onto waste tea residue: kinetic, equilibrium, breakthrough and reusability studies. Journal of Cleaner Production. 2020;252:119778. https://doi.org/10.1016/j.jclepro.2019.119778
2. 2. Darban AK, Shahedi A, Taghipour F, Jamshidi-Zanjani A. A review on industrial wastewater treatment via electrocoagulation processes. Current Opinion in Electrochemistry. 2020; 22:154–169. https://doi.org/10.1016/j.coelec.2020.05.009.
3. 3. Trojanowicz M. Removal of persistent organic pollutants (POPs) from waters and wastewaters by the use of ionizing radiation. Science of Total Environonment. 2020;718:134425. https://doi.org/10.1016/j.scitotenv.2019.134425
4. 4. Huerta-Fontela M, Galceran MT, Ventura F. Occurrence and removal of pharmaceuticals and hormones through drinking water treatment. Water Research. 2011;45:1432-1442. https://doi.org/10.1016/j.watres.2010.10.036
5. 5. Li Y, Zhu G, Ng WJ, Tan SK. A review on removing pharmaceutical contaminants from wastewater by constructed wetlands: design, performance and mechanism. Science of The Total Environment. 2014;468–469:908–932. https://doi.org/10.1016/j.scitotenv.2013.09.018
6. 6. EU 2008. European Union. Water framework directive 2008/105/EC. European parliament and of the council. [cited 20 August 2016]. Available from: http://eur-lex.europa.eu/legal-content/EN/TXT/?uri=CELEX:32008L0105.
7. 7. Kostich MS, Batt AL, Lazorchak JM. Concentrations of prioritized pharmaceuticals in effluents from 50 large wastewater treatment plants in the US and implications for risk estimation. Environmental Pollution. 2014;184:354–359. https://doi.org/10.1016/j.envpol.2013.09.013
8. 8. Bartels P, von Tümpling W. Solar radiation influence on the decomposition process of diclofenac in surface waters. Science of the Total Environmet. 2007;374(1):143-155. https://doi.org/10.1016/j.scitotenv.2006.11.039

9. 9. Alvarez S, Ribeiro RS, Gomes HT, Sotelo JL, García J. Synthesis of carbon xerogels and their application in adsorption studies of caffeine and diclofenac as emerging contaminants. Chemical Engineering Research Design. 2015;95:229-238. https://doi.org/10.1016/j.cherd.2014.11.001
10. 10. Acuña V, Ginebred A, Mor JR, Petrovic M, Sabater S, Sumpter J, Barceló D. Balancing the health benefits and environmental risks of pharmaceuticals: diclofenac as an example. Environment International. 2015;85:327–333.
11. 11. Bhadra BN, Ahmed I, Kim S, Jhung SH. Adsorptive removal of ibuprofen and diclofenac from water using metal-organic framework-derived porous carbon. Chemical Engineering Journal. 2017;314:50-58. https://doi.org/10.1016/j.cej.2016.12.127
12. 12. Margot J, et al.Treatment of micropollutants in municipal wastewater: ozone or powdered activated carbon. Science of the Total Environment. 2013;461–462:480–498. https://doi.org/10.1016/j.scitotenv.2013.05.034
13. 13. Huang Z, Gong B, Huang C-P, et al. Performance evaluation of integrated adsorption-nanofiltration system for emerging compounds removal: Exemplified by caffeine, diclofenac and octylphenol. Journal of Environmental Management. 2019;231:121-128. https://doi.org/10.1016/j.jenvman.2018.09.092
14. 14. Lima FS, de Barros Neto EL, Melo RPF, et al. Removal of diclofenac sodium from aqueous solution using ionic micellar flocculation-assisted adsorption. Separation Science and Technology. 2022;57:2997-3011. https://doi.org/10.1080/01496395.2022.2085577
15. 15. Rigobello ES, Dantas ADB, Bernado LD, Vieira EM. Removal of diclofenac by conventional drinking water treatment processes and granular activated carbon filtration. Chemosphere. 2013;92:184-191. https://doi.org/10.1016/j.chemosphere.2013.03.010
16. 16. Suarez S, Lema JM, Omil F. Pre-treatment of Hospital Wastewater by Coagulation– Flocculation and Flotation. Bioresource Technology. 2009;100(7):2138–2146. https://doi.org/10.1016/j.biortech.2008.11.015
17. 17. Marcela AEF, Cassandra BC, Mariana MB. Rafael de PS. Liliana AF. Diclofenac removal from water by adsorption using activated carbon in batch mode and fixed-bed column: Isotherms, thermodynamic study and breakthrough curves modeling. Journal of Cleaner Production. 2018;181:145-154. https://doi.org/10.1016/j.jclepro.2018.01.138
18. 18. Kennedy AM, Reinert AM, Knappe DRU, Ferrer I, Summers RS. Fulland pilot-scale GAC adsorption of organic micropollutants. Water Research. 2015;68:238-248. https://doi.org/10.1016/j.watres.2014.10.010
19. 19. Moreira NFF, Orge CA, Ribeiro AR, Faria JL, Nunes OC, Pereira MFR, Silva AMT. Fast mineralization and detoxification of amoxicillin and diclofenac by photocatalytic ozonation and application to an urban wastewater. Water Res. 2017; 87: 87-96. https://doi.org/10.1016/j.watres.2015.08.059
20. 20. Phattarapattamawong S, Kaiser AM, Saracevic E, Schaar HP, Krampe J. Optimization of ozonation and peroxone process for simultaneous control of micropollutants and bromate in wastewater. Water Science and Technology. 2018;2:404–411. https://doi.org/10.2166/wst.2018.170
21. 21. Ozdemir K. The use of carbon nanomaterials for removing natural organic matter in drinking water sources by a combined coagulation process. Nanomaterials and Nanotechnology. 2016;6:1-12. https://doi.org/10.1177/1847980416663680
22. 22. Wang X, Lu J, Xing B. Sorption of organic contaminants by carbon nanotubes: Influence of adsorbed organic matter. Environonmental Science Technology. 2008;42:3207–3212. https://doi.org/10.1021/es702971g
23. 23. Özdemir K. Removal of Arsenate in Drinking Water Sources by Combined Coagulation Process. Journal of the Turkish Chemical Society Section A: Chemistry. 2022;9(1):247-254. https://doi.org/10.18596/jotcsa.980203
24. 24. APHA. Standard methods for the examination of water and waste water. Washington, 21st ed.DC: American Public Health Assoc. 2005.
25. 25. Zhao J, Xu L, Su Y, Yu H, Liu H, Qian S, Zheng W, Zhao Y. Zr-MOFs loaded on polyurethane foam by polydopamine for enhanced dye adsorption. Jorunal of Environmental Science. 2021;101:177–188. https://doi.org/10.1016/j.jes.2020.08.021.
26. 26. Fatima ET, Hicham Z, Hanane A, Jamila ElG, Rachid AA, Mohamed H. Removal of Persistent Organic Pollutants (POPs) from water and wastewater by adsorption and electrocoagulation process. Groundwater Sustainable Development. 2021;13:1-23. https://doi.org/10.1016/j.gsd.2021.100575
27. 27. Humbert H, Gallard H, Suty H. Natural organic matter(NOM) and pesticides removal using a combination of ion exchange resin and powdered activated carbon (PAC). Water Research. 2008;42:1635–1643. https://doi.org/10.1016/j.watres.2007.10.012
28. 28. Bolto B, Dixon D, Eldridge R. Removal of natural organic matter by ion exchange. Water Research. 2002;36:5057–5065. https://doi.org/10.1016/S0043-1354(02)00231-2
29. 29. Rashid MA, Buckley DE, Robertson KR. Interactions of a marine humic acid with clay minerals and natural sedimen. Geoderma. 1972;8:11–27. https://doi.org/10.1016/0016-7061(72)90029-8
30. 30. Fontecha-Camara MA, Lopez-Ramon MV, Alvarez-Merino MA, Moreno-Castilla C. Effect of surface chemistry, solution pH, and ionic strength on the removal of herbicides diuron and amitrole from water by an activated carbon fiber. Langmuir. 2007;23:1242–1247. https://doi.org/10.1021/la062200f
31. 31. Vinu A, Hossain KZ, Kumar GS, Ariga K. Adsorption of L-histidine over mesoporous carbon molecular sieves. Carbon. 2006;44:530–536.
32. 32. Yousef RI, El-Eswed B, Al-Muhtaseb AH. Adsorption characteristics of natural zeolites as solid adsorbents for phenol removal from aqueous solutions: kinetics, mechanism, and thermodynamics studies. Chemical Engineering Journal. 2011;171 (3):1143-1149. https://doi.org/10.1016/j.cej.2011.05.012
33. 33. Pezoti O, Cazetta AL, Bedin KC, Souza LS, Martins AC, Silva TL, Santos Júnior OO, Visentainer JV, Almeida VC. NaOH-activated carbon of high surface area produced from guava seeds as a high-efficiency adsorbent for amoxicillin removal: kinetic, isotherm and thermodynamic studies. Chemical Engineering Journal. 2016;288:778-788. https://doi.org/10.1016/j.cej.2015.12.042
34. 34. Jodeh S, Abdelwahab F, Jaradat N, Warad I, Jodeh W. Adsorption of diclofenac from aqueous solution using Cyclamen persicum tubers based activated carbon (CTAC). Journal of the Association Arab. Universities for Basic and Applied Sciences. 2014. https://doi.org/10.1016/j.jaubas.2014.11.002
35. 35. Sotelo JL, Ovejero G, Rodríguez A, Alvarez S, Galan J, García J. Competitive adsorption studies of caffeine and diclofenac aqueous solutions by activated carbon. Chemical Engineering Journal. 2014;240:443-453. https://doi.org/10.1016/j.cej.2013.11.094
36. 36. Zhao Y, Liu F, Qin X. Adsorption of diclofenac onto goethite: adsorption kinetics and effects of pH. Chemosphere. 2017;180:373-378. https://doi.org/10.1016/j.chemosphere.2017.04.007