The effect of physicochemical properties on paracetamol photodegradation in cuboid bubble column

Abstract

Paracetamol is one of the most anthropogenic micropollutants, and their removal from the environment often requires a specialized method of remediation. In this study, a photocatalyst technique aided with air bubbles was used to degrade the pharmaceutical pollutant paracetamol (PCT) from the water via the COD test and HPLC analysis under different operating conditions. The experiments were carried out in a semi-batch rectangular bubble column with dimensions of 1500 mm height, 30 mm depth, and 200 mm width under UV light. Titanium oxide (TiO2) was used as a source of catalyst. The effect of operating conditions of pH (3-10), air flow rate (0-2) L/min, salinity of solution represented by NaCl concentration (0-1000) mg/L, and 240 min irradiation time on the paracetamol removal were studied. The Box–Behnken design was adopted to study the individual effects of pH (A), air flow rate (B), and salinity (C) and their interactive effects. From the experimental and regression data, a second-order polynomial regression model is predicted, and the variance analysis of the regressions shows that the linear terms (A and B), and all quadratic terms (A, B, and C) have significant effects on the removal percentage of COD. According to numerical optimization, the greatest %COD removal is 76.7 in the process conditions of 5.3 pH, 1L/min, and 269 mg/L of NaCl. The experimental results show that the maximum %COD removal was 78% at pH=7, 1L/min, and 0mg/L of NaCl. HPLC analysis shows 91.2% of paracetamol degradation.

Keywords

• Pharmaceuticals
• photocatalyst
• response surface modelin
• titanium dioxide

References

1. C. Gadipelly, A. Pérez-González, G. D. Yadav, I. Ortiz, R. Ibáñez, V. K. Rathod, and K. V. Marathe, “Pharmaceutical ındustry wastewater: Review of the technologies for water treatment and reuse,” Industrial & Engineering Chemistry Research, Vol. 53(29), pp. 11571-11592, 2014. [CrossRef]
2. A. R. Ribeiro, O. C. Nunes, M. F. R. Pereira, and A. M. T. Silva, “An overview of the advanced oxidation processes applied for the treatment of water pollutants defined in the recently launched directive 2013/39/EU,” Environmental International, Vol. 75, pp. 33-51, 2015. [CrossRef]
3. T. Heberer, “Tracking persistent pharmaceutical residues from municipal sewage to drinking water,” Journal of Hydrology, Vol. 266(3–4), pp. 175–189, 2002. [CrossRef]
4. C. Tixier, H. P. Singer, S. Oellers, and S. R. Müller, “Occurrence and fate of carbamazepine, clofibric acid, diclofenac, ıbuprofen, ketoprofen, and naproxen in surface waters,” Environmental Science & Technology, Vol. 37(6), pp. 1061–1068, 2003. [CrossRef]
5. K. Fent, A. A. Weston, and D. Caminada, “Ecotoxicology of human pharmaceuticals,” Aquatic Toxicology, Vol. 76(2), pp. 122–159, 2006. [CrossRef]
6. C. Miege, J. M. Choubert, L. Ribeiro, M. Eusebe, and M. Coquery, “Fate of pharmaceuticals and personal care products in wastewater treatment plants—conception of a database and first results,” Environmental Pollution, Vol. 157(5), pp. 1721–1726, 2008. [CrossRef]
7. K. Kümmerer, “The presence of pharmaceuticals in the environment due to human use-present knowledge and future challenges,” Journal of Environmental Management, Vol. 90(8), pp. 2354–2366, 2009. [CrossRef]
8. S. Mompelat, B. Le Bot, and O. Thomas, “Occurrence and fate of pharmaceutical products and by-products, from resource to drinking water,” Environmental International, Vol. 35(5), pp. 803–814, 2009. [CrossRef]

9. I. M. Sebastine, and R. J. Wakeman, “Consumption and environmental hazards of pharmaceutical substances in the UK,” Process Safety and Environmental Protection, Vol. 81(B4), pp. 229-235, 2003. [CrossRef]
10. L. Yang, L. E. Yu, and M. B. Ray, “Degradation of paracetamol in aqueous solutions by TiO2 photocatalysis,” Water Research, Vol. 42(13), pp. 3480-3488, 2008. [CrossRef]
11. B. C. Lourenção, R. A. Medeiros, R. C. Rocha-Filho, L. H. Mazo, and O. Fatibello-Filho, “Simultaneous voltammetric determination of paracetamol and caffeine in pharmaceutical formulations using a boron-doped diamond electrode,” Talanta, Vol. 78(3), pp. 748–752, 2009. [CrossRef]
12. M. Solé, J. P. Shaw, P. E. Frickers, J. W. Readman, and T. H. Hutchinson, “Effects on feeding rate and biomarker responses of marine mussels experimentally exposed to propranolol and acetaminophen,” Analytical and Bioanalytical Chemistry, Vol. 96, pp. 649–656, 2010. [CrossRef]
13. K. H. Langford, and K. V. Thomas, “Determination of pharmaceutical compounds in hospital effluents and their contribution to wastewater treatment works,” Environment International, Vol. 35(5), pp. 766-770, 2009. [CrossRef]
14. P. J. Phillips, S. G. Smith, D. W. Kolpin, S. D. Zaugg, H. T. Buxton, E. T. Furlong, K. Esposito, and B. Stinson, “Pharmaceutical formulation facilities as sources of opioids and other pharmaceuticals to wastewater treatment plant effluents,” Environmental Science & Technology, Vol. 44(13), pp. 4910–4916, 2010. [CrossRef]
15. J. J. Xu, B. S. Hendriks, J. Zhao, and D. Graaf, “Multiple effects of acetaminophen and p38 ınhibitors: towards pathway toxicology,” FEBS Letters, Vol. 582, pp. 1276–1282, 2008. [CrossRef]
16. A. Carabin, P. Drogui, and D. Robert, “Photo-degradation of carbamazepine using TiO2 suspended photocatalysts,” Journal of the Taiwan Institute of Chemical Engineers, Vol. 54, pp. 109-117, 2015. [CrossRef]
17. N. Muir, J. D. Nichols, M. R. Stillings, and J. Sykes, “Comparative bioavailability of aspirin and paracetamol following single dose administration of soluble and plain tablets,” Current Medical Research and Opinion, Vol. 13(9), pp. 491-500, 1997. [CrossRef]
18. J. Wang, and S. Wang, “Removal of pharmaceuticals and personal care products (PPCPs) from wastewater: A review,” Journal of Environmental Management, Vol. 182, pp. 620–640, 2016. [CrossRef]
19. M. Chen, F. Zhang, C. Cui, X. Liao, J. Chen, J. Rong, and D. Yu, “Treatment of wastewater from paracetamol factory by using non-thermal plasma and active carbon,” Materials for Renewable Energy and Environment, 2011 International Conference on Materials for Renewable Energy & Environment, 2011. [CrossRef]
20. U. Nielsen, C. Hastrup, M. M. Klausen, B. M. Pedersen, G. H. Kristensen, J. L. C. Jansen, S. N. Bak, and J. Tuerk, “Removal of APIs and bacteria from hospital wastewater by MBR plus O3, O3 + H2O2, PAC or ClO2,” Water Science and Technology, Vol. 67, pp. 854–862, 2013. [CrossRef]
21. Y. Mameri, N. Debbache, M. E. M. Benacherine, N. Seraghni, and T. Sehili, “Heterogeneous Photodegradation of Paracetamol using Goethite/H2O2 and Goethite/oxalic acid systems under artificial and natural light,” Journal of Photochemistry and Photobiology A: Chemistry, Vol. 315, pp. 129-137, 2016. [CrossRef]
22. M. E. M. Benacherine, N. Debbache, I. Ghoul, and Y. Mameri, “Heterogeneous photoinduced degradation of amoxicillin by goethite under artificial and natural irradiation,” Journal of Photochemistry and Photobiology A: Chemistry, Vol. 335, pp. 70-77, 2017. [CrossRef]
23. H. Al Qarni, P. Collier, J. O’Keeffe, and J. Akunna, “Investigating the removal of some pharmaceutical compounds in hospital wastewater treatment plants operating in Saudi Arabia,” Environmental Science and Pollution Research, Vol. 23, pp. 13003–13014, 2016. [CrossRef]
24. G. Dalgıç, F. Ilter Turkdogan, K. Yetilmezsoy, and E. Kocak, “Treatment of real paracetamol wastewater by Fenton process,” Chemical İndustry and Chemical Engineering, Vol. 23(2), pp. 177-186, 2016. [CrossRef]
25. C. M. Lee, P. Palaniandy, N. Q. Zaman, and M. N. Adlan “Pharmaceutical removal from synthetic wastewater using heterogeneous – photocatalyst,” Applied Mechanics and Materials, Vol. 802, pp. 507-512, 2015. [CrossRef]
26. J. P. Scott, and D. F. Ollis, “Integration of chemical and biological oxidation processes for water treatment” Environmental Progress, Vol. 14, pp. 88–103, 1995. [CrossRef]
27. I. K. Konstantinou, and T. A. Albanis, “TiO2-assisted photocatalytic degradation of azo dyes in aqueous solution: kinetic and mechanistic investigations – a review,” Applied Catalysis B: Environmental, Vol. 49, pp. 1–14, 2004. [CrossRef]
28. M. A. Al-Nuaim, A. A. Al-Wasiti, Z. Y. Shnain, and A. K. Al-Shalal, “The combined effect of bubble and photo catalysis technology in BTEX removal from produced water,” Bulletin of Chemical Reaction Engineering & Catalysis, Vol. 17(3), pp. 577-589 2022. [CrossRef]
29. N. E. Mousa, S. Seba, Z. Yousif, M. Abid, A. Alwasiti, and K. Sukkar, “Catalytic photodegradation of cyclic sulfur compounds in a model fuel using a bench-scale falling-film reactor ırradiated by a visible light,” Bulletin of Chemical Reaction Engineering & Catalysis, Vol. 17(4), pp. 755-767, 2022. [CrossRef]
30. H. Shemer, Y. K. Kunukcu, and K. G. Linden, “Degradation of the pharmaceutical metronidazole via UV, Fenton and photo-Fenton processes,” Chemosphere, Vol. 63, pp. 269–276, 2005. [CrossRef]
31. S. A. Abdulrahman, S. S. Ibraheem, and Z. Y. Shnain, “An overview of wastewater treatment using combined heterogeneous photocatalysis and membrane distillation,” Chimica Techno Acta, Vol. 10(1), 202310114, 2023. [CrossRef]
32. A. K. Majhool, K. A. Sukkar, and M. A. Alsaffar, “Combining α-Al2O3 packing material and a ZnO nanocatalyst in an ozonized bubble column reactor to ıncrease the phenol degradation from wastewater,” Processes, Vol. 11, Article 2416, 2023. [CrossRef]
33. Y. Cheng, H. Sun, W. Jin, and N. Xu, “Photocatalytic degradation of 4-chlorophenol with combustion synthesized TiO2 under visible light irradiation,” Chemical Engineering Journal, Vol. 128, pp. 127–133, 2007. [CrossRef]
34. S. A. Abdulrahman, Z. Y. Shnain, S. S. Ibrahim, and H. S. Majdi, “Photocatalytic degradation of ciprofloxacin by UV light using n-doped TiO2 in suspension and coated forms,” Catalysts, Vol. 12, Article 1663, 2022. [CrossRef]
35. F.S. Freyria, M. Armandi, M. Compagnoni, G. Ramis, I. Rossetti, and B. Bonelli, “Catalytic and photocatalytic processes for the abatement of n-containing pollutants from wastewater. part 2: Organic pollutants,” Journal of Nanoscience and Nanotechnology, Vol. 17, pp. 3654–3672, 2017.
36. M. Compagnoni, G. Ramis, F.S. Freyria, M. Armandi, B. Bonelli, and I. Rossetti, “Photocatalytic processes for the abatement of n-containing pollutants from wastewater. Part 1: Inorganic pollutants,” Journal of Nanoscience and Nanotechnology, Vol. 17, pp. 3632–3653, 2017.
37. N. Blangetti, F. S. Freyria, M. C. Calviello, N. Ditaranto, S. Guastella, and B. Bonelli, “Photocatalytic degradation of paracetamol under simulated sunlight by four TiO2 commercial powders: An ınsight into the performance of two sub-micrometric anatase and rutile powders and a nanometric brookite powder,” Catalysts, Vol. 13(2), Article 434, 2023.
38. M. A. Al-Nuaim, A. A. Alwasiti, and Z. Y. Shnain, “The photocatalytic process in the treatment of polluted water,” Chemical Papers, Vol. 77, pp. 677–701, 2023.
39. K.-H. Wang, Y.-H. Hsieh, C.-H. Wu, and C.-Y. Chang, “The pH and anion effects on the heterogeneous photocatalytic degradation of o-methylbenzoic acid in TiO2 aqueous suspension,” Chemosphere, Vol. 40(4), 389-394, 2000.
40. H.Y. Chen, O. Zahraa, and M. Bouchy, “Inhibition of the adsorption and photocatalytic degradation of an organic contaminant in an aqueous suspension of TiO_2 by inorganic ions,” Journal of Photochemistry and Photobiology A: Chemistry, Vol. 108, Article 37, 1997.
41. J. P. Holmberg, E. Ahlberg, J. Bergenholtz, M. Hassellöv, and Z. Abbas, “Surface charge and interfacial potential of titanium dioxide nanoparticles: Experimental and theoretical investigations,” Journal of Colloid and Interface Science, Vol. 407, pp. 168–176, 2013.
42. N. Jallouli, K. Elghniji, H. Trabelsi, and M. Ksibi, “Photocatalytic degradation of paracetamol on TiO2 nanoparticles and TiO2/cellulosic fiber under UV and sunlight irradiation,” Arabian Journal of Chemistry, Vol. 10(Suppl 2), pp. S3640-S3645, 2017.
43. T. M. A. Dalmázio, R. Alves, and R. Augusti, “An appraisal on the degradation of paracetamol by TiO2/UV system in aqueous medium. Product identification by gas chromatography–mass spectrometry,” Journal of the Brazilian Chemical Society, Vol. 19(1), pp. 81–88, 2008.
44. A. Sclafani, L. Palmisano, and E. Davi, “Photocatalytic degradation of hydroxyethylcellulose in aqueous Pt TiO_2 suspension,” Journal of Photochemistry and Photobiology A: Chemistry, Vol. 56, Article 113, 1991.
45. M. Fujihira, Y. Satoh, and T. Osa, “Photocatalytic degradation of organic water contaminants: Mechanisms involving hydroxyl radical attack,” Bulletin of Chemical Reaction Engineering & Catalysis, Vol. 66, 1982.
46. C. Kormann, D. W. Bahnemann, and M. R. Hoffmann, “Photolysis of chloroform and other organic molecules in aqueous titanium dioxide suspensions,” Environmental Science & Technology, Vol. 25, pp. 494-499, 1991.
47. D. F. Ollis, C. Y. Hsiar, L. Budiman, and C. L. Lee, “Visible-light activation of TiO2 photocatalysts: Advances in theory and experiments,” Journal of Photochemistry and Photobiology C: Photochemistry Reviews, Vol. 25, pp. 1-29, 2015.
48. C. Maillard-Dupuy, C. Guillard, and P. Pichat, “Kinetics and products of the TiO2 photocatalytic degradation of pyridine in water,” New Journal of Chemistry, Vol. 18, pp. 941-945, 1994.
49. E. Mostafa, P. Reinsberg, S. Garcia-Segura, and H. Baltruschat, “Chlorine species evolution during electrochlorination on boron-doped diamond anodes: In-situ electrogeneration of Cl2, Cl2O and ClO2,” Electrochimica Acta, Vol. 281, pp. 831-840, 2018.
50. N. Jallouli, K. Elghniji, H. Trabelsi, and M. Ksibi, “Photocatalytic degradation of paracetamol on TiO2 nanoparticles and TiO2/cellulosic fiber under UV and sunlight irradiation,” Arabian Journal of Chemistry, 2014.
51. A. Abdelhaleem, H. N. Abdelhamid, M. G. Ibrahim, and W. Chu, "Photocatalytic degradation of paracetamol using photo-Fenton-like metal-organic framework-derived CuO@C under visible LED," Journal of Cleaner Production, Vol. 379, 2022, 134571. DOI: 10.1016/j.jclepro.2022.134571.
52. D. C. S. Gloria, C. H. V. Brito, T. A. P. Mendonça, T. R. Brazil, R. A. Domingues, N. C. S. Vieira, E. B. Santos, and M. Gonçalves, "Preparation of TiO2/activated carbon nanomaterials with enhanced photocatalytic activity in paracetamol degradation," Materials Chemistry and Physics, Vol. 305, 127947, 2023. DOI: 10.1016/j.matchemphys.2023.127947.