Springer Nature is making SARS-CoV-2 and COVID-19 research free. View research | View latest news | Sign up for updates

Optimization of photocatalytic degradation of meloxicam using titanium dioxide nanoparticles: application to pharmaceutical wastewater analysis, treatment, and cleaning validation

Abstract

Meloxicam is a commonly prescribed nonsteroidal anti-inflammatory drug with analgesic and fever-reducing effects. In this study, photocatalytic degradation of meloxicam in the presence of TiO2 nanoparticles (TiO2NP) was optimized and applied for pharmaceutical wastewater treatment. A validated stability-indicating orthogonal testing protocol (reversed-phase (RP)-HPLC and capillary zone electrophoresis) was developed and validated for monitoring of meloxicam concentration in the presence of its photodegradation products. Fractional factorial design was employed in order to investigate the effects of pH, irradiation time, UV light intensity, TiO2NP loading, and initial meloxicam concentration on the efficiency of the process. The light intensity was found as the most significant parameter followed by irradiation time and concentration, respectively. The most influencing interactions were noted between irradiation time–concentration and irradiation time–light intensity. The kinetics of meloxicam degradation was investigated at the optimum set of experimental conditions. The protocol was successfully applied for treatment of incurred water samples collected during various cleaning validation cycles. A percentage degradation of 77.34 ± 0.02 % was achieved upon irradiation of samples containing 64.57 ± 0.09 μg/mL with UV light (1012 μW/cm2, 8 h) in the presence of 0.4 mg/mL TiO2NP at pH 9.0 ± 0.05. Treatment of wastewaters collected during the cleaning validation of each product separately rather than the combined waste should result in a significant improvement in the economics of pharmaceutical wastewater treatment. This could be attributed to the relatively small waste volumes and the ability to tailor the experimental conditions to achieve maximum efficiency.

This is a preview of subscription content, log in to check access.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5

References

  1. Al-Ghobashy MA (2014) Electrophoretic behavior of charge regulated zwitterionic buffers in covalently and dynamically coated fused silica capillaries. Bull Faculty Pharm CU 52:71–78

  2. Al-Ghobashy MA, Williams MAK, Laible G, Harding DRK (2011) CZE with on-line micellar sample stacking for determination of protein concentration of biopharmaceuticals. Chromatographia 73:1145–1153

  3. Altınoz S, Nemutlu E, Kır S (2002) Polarographic behaviour of meloxicam and its determination in tablet preparations and spiked plasma Il. Farmaco 57:463–468

  4. Ammar S, Oturan MA, Labiadh L, Guersalli A, Abdelhedi R, Oturan N, Brillas E (2015) Degradation of tyrosol by a novel electro-Fenton process using pyrite as heterogeneous source of iron catalyst. Water Res 74:77–87

  5. Anglada A, Urtiaga A, Ortiz I (2009) Contributions of electrochemical oxidation to waste‐water treatment: fundamentals and review of applications. J Chem Technol Biotechnol 84:1747–1755

  6. Bae J-W, Kim M-J, Jang C-G, Lee S-Y (2007) Determination of meloxicam in human plasma using a HPLC method with UV detection and its application to a pharmacokinetic study. J Chromatogr B 859:69–73

  7. British Pharmacopoeia (2007) The Council of Europe, France

  8. Calza P, Sakkas V, Medana C, Baiocchi C, Dimou A, Pelizzetti E, Albanis T (2006) Photocatalytic degradation study of diclofenac over aqueous TiO2 suspensions. Appl Catal B Environ 67:197–205

  9. Carballa M, Omil F, Lema JM (2005) Removal of cosmetic ingredients and pharmaceuticals in sewage primary treatment. Water Res 39:4790–4796

  10. Chong MN, Jin B, Chow CW, Saint C (2010) Recent developments in photocatalytic water treatment technology: a review. Water Res 44:2997–3027

  11. Duan F, Li Y, Cao H, Wang Y, Crittenden JC, Zhang Y (2015) Activated carbon electrodes: electrochemical oxidation coupled with desalination for wastewater treatment Chemosphere

  12. Giraldo AL, Penuela GA, Torres-Palma RA, Pino NJ, Palominos RA, Mansilla HD (2010) Degradation of the antibiotic oxolinic acid by photocatalysis with TiO2 in suspension. Water Res 44:5158–5167

  13. Gros M, Rodríguez-Mozaz S, Barcelo D (2012) Fast and comprehensive multi-residue analysis of a broad range of human and veterinary pharmaceuticals and some of their metabolites in surface and treated waters by ultra-high-performance liquid chromatography coupled to quadrupole-linear ion trap tandem mass spectrometry. J Chromatogr A 1248:104–121

  14. Hassan EM (2002) Spectrophotometric and fluorimetric methods for the determination of meloxicam in dosage forms. J Pharm Biomed Anal 27:771–777

  15. Huerta-Fontela M, Galceran MT, Ventura F (2011) Occurrence and removal of pharmaceuticals and hormones through drinking water treatment. Water Res 45:1432–1442

  16. ICH Guidelines:Q2(R1) Validation of analytical procedures (2005)

  17. Kim SD, Cho J, Kim IS, Vanderford BJ, Snyder SA (2007) Occurrence and removal of pharmaceuticals and endocrine disruptors in South Korean surface, drinking, and waste waters. Water Res 41:1013–1021

  18. Konstantyinou IK, Albanis TA (2004) TiO2-assisted photocatalytic degradation of azo dyes in aqueous solution: kinetic and mechanistic investigations: a review. App Catal B: Environmental 49:1–14

  19. Lin Y, Ferronato C, Deng N, Wu F, Chovelon J-M (2009) Photocatalytic degradation of methylparaben by TiO2: multivariable experimental design and mechanism. Appl Catal B: Environmental 88:32–41

  20. Malato S, Blanco J, Vidal A, Richter C (2002) Photocatalysis with solar energy at a pilot-plant scale: an overview. Appl Catal B: Environmental 37:1–15

  21. Marotta R, Spasiano D, Di Somma I, Andreozzi R (2013) Photodegradation of naproxen and its photoproducts in aqueous solution at 254 nm: a kinetic investigation. Water Res 47:373–383

  22. Mendez-Arriaga F, Esplugas S, Gimenez J (2008) Photocatalytic degradation of non-steroidal anti-inflammatory drugs with TiO2 and simulated solar irradiation. Water Res 42:585–594

  23. Modhave DT, Handa T, Shah RP, Singh S (2011) Successful characterization of degradation products of drugs using LC-MS tools: application to piroxicam and meloxicam. Anal Methods 3:2864–2872

  24. Nakata K, Fujishima A (2012) TiO2 photocatalysis: design and applications. J Photochem Photobiol C: Photochemistry Rev 13:169–189

  25. Nemutlu E, Kir S (2003) Method development and validation for the analysis of meloxicam in tablets by CZE. J Pharm Biomed Anal 31:393–400

  26. Palominos RA, Mondaca MA, Giraldo A, Penuela G, Perez-Moya M, Mansilla HD (2009) Photocatalytic oxidation of the antibiotic tetracycline on TiO2 and ZnO suspensions. Catal Today 144:100–105

  27. Qu X, Alvarez PJ, Li Q (2013) Applications of nanotechnology in water and wastewater treatment. Water Res 47:3931–3946

  28. Sakkas VA, Islam MA, Stalikas C, Albanis TA (2010) Photocatalytic degradation using design of experiments: a review and example of the Congo red degradation. J Hazard Mater 175:33–44

  29. Seedher N, Bhatia S (2003) Solubility enhancement of Cox-2 inhibitors using various solvent systems. AAPS Pharm Sci Tech 4:36–44

  30. Sires I, Brillas E (2012) Remediation of water pollution caused by pharmaceutical residues based on electrochemical separation and degradation technologies: a review. Environ Int 40:212–229

  31. Starek M, Krzek J (2009) A review of analytical techniques for determination of oxicams, nimesulide and nabumetone. Talanta 77:925–942

  32. The United States Pharmacopoeia & National Formulary (2011) US Pharmacopoeial Convention Inc., USA

  33. Velpandian T, Jaiswal J, Bhardwaj RK, Gupta SK (2000) Development and validation of a new high-performance liquid chromatographic estimation method of meloxicam in biological samples. J Chromatogr B 738:431–436

  34. Yang L, Yu LE, Ray MB (2008) Degradation of paracetamol in aqueous solutions by TiO2 photocatalysis. Water Res 42:3480–3488

Download references

Author information

Correspondence to Medhat A. Al-Ghobashy.

Additional information

Responsible editor: Philippe Garrigues

Electronic supplementary material

Below is the link to the electronic supplementary material.

ESM 1

(DOCX 218 kb)

Rights and permissions

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

Nadim, A.H., Al-Ghobashy, M.A., Nebsen, M. et al. Optimization of photocatalytic degradation of meloxicam using titanium dioxide nanoparticles: application to pharmaceutical wastewater analysis, treatment, and cleaning validation. Environ Sci Pollut Res 22, 15516–15525 (2015). https://doi.org/10.1007/s11356-015-4713-2

Download citation

Keywords

  • Pharmaceutical wastewater treatment
  • Cleaning validation
  • RP-HPLC
  • Photodegradation
  • Titanium dioxide nanoparticles