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Assessment of integrated binary process by coupling photocatalysis and photo-Fenton for the removal of cephalexin from aqueous solution

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Abstract

A novel concept of integrated process by coupling photocatalysis and photo-Fenton especially in fixed mode has been presented in the current study for the removal of recalcitrant pharmaceuticals like cephalexin (CEX) from aqueous solution in reduced treatment time. Waste materials like foundry sand (FS) was used as a substitute for iron along with TiO2. The parametric optimization was carried out in slurry mode using Box–Behnken design model (BBD) and response surface methodology. For fixed-bed studies, support materials of varying shapes (hollow circular disk, rectangular slabs, spherical beads) were prepared using clay in conjunction with FS for TiO2 immobilization. Different supports were compared on the basis of degradation efficiency, exposed surface area of catalyst as well as their recyclability capacity for the degradation of CEX. Iron was leaching by default from the supports during the degradation process which contributed simultaneously to photo-Fenton process along with photocatalysis. Spherical beads with 0.0265 m2 exposed surface area of catalyst and better recyclability efficiency (10 cycles) yielded best degradation efficiency (80%) of CEX after 240 min of treatment time. The presence of iron along with TiO2 on the surface of beads was confirmed through TGA, SEM/EDS, XRD, DRS and FTIR. The mineralization of CEX was validated through quantification of nitrite, nitrate and sulfate ions along with reduction in COD. A tentative pathway for the degradation of CEX was also proposed based on the identification of intermediates through GC–MS analysis.

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References

  1. Díaz-Cruz MS, Barceló D (2008) Trace organic chemicals contamination in ground water recharge. Chemosphere 72:333–342

    Article  Google Scholar 

  2. Piscopo A, Robert D, Marzolin C, Weber JV (2000) TiO2 supported on glass fiber for the photocatalytic degradation of benzamide. J Mat Sci Lett 19:683–684

    Article  Google Scholar 

  3. Pettit SL, Rodriguez-Gonzalez L, Michaels JT, Alcantar NA, Ergas SJ, Kuhn JN (2014) Parameters influencing the photocatalytic degradation of geosmin and 2-methylisoborneol utilizing immobilized TiO2. Catal Lett 144:1460–1465

    Article  Google Scholar 

  4. Yogi C, Kojima K, Takai T, Wada N (2009) Photocatalytic degradation of methylene blue by Au-deposited TiO2 film under UV irradiation. J Mat Sci 44:821

    Article  Google Scholar 

  5. Bansal P, Verma A, Aggarwal K, Singh A, Gupta S (2016) Investigations on the degradation of an antibiotic Cephalexin using suspended and supported TiO2: mineralization and durability studies. Can J Chem Eng 94:1269–1276

    Article  Google Scholar 

  6. Shi T, Peng J, Chen J, Sun C, He H (2017) Heterogeneous photo-fenton degradation of norfloxacin with Fe3O4-multiwalled carbon nanotubes in aqueous solution. Catal Lett 147:1598–1607

    Article  Google Scholar 

  7. Verma A, Dixit D, Toor A, Srivastava J (2015) Heterogeneous photocatalytic degradation of 2-chloro-4-nitrophenol using slurry and fixed bed reactor. Environ Prog Sustain Energy 34:380–386

    Article  Google Scholar 

  8. Blanco E, González-Leal JM, Ramírez-del M (2015) Photocatalytic TiO2 sol–gel thin films: optical and morphological characterization. Sol Energy 122:11–23

    Article  Google Scholar 

  9. Ramirez JH, Maldonado-Hódar FJ, Pérez-Cadenas AF, Moreno-Castilla C, Costa CA, Madeira LM (2007) Azo-dye orange II degradation by heterogeneous Fenton-like reaction using carbon-Fe catalysts. Appl Catal B 75:312–323

    Article  Google Scholar 

  10. Samarghandi MR, Nouri J, Mesdaghinia AR, Mahvi AH, Nasseri S, Vaezi F (2007) Efficiency removal of phenol, lead and cadmium by means of UV/TiO2/H2O2 processes. Int J Environ Sci Technol 4:19–25

    Article  Google Scholar 

  11. Mazille F, Schoettl T, Pulgarin C (2009) Synergistic effect of TiO2 and iron oxide supported on fluorocarbon films. Part 1: effect of preparation parameters on photocatalytic degradation of organic pollutant at neutral pH. Appl Catal B Environ 89:635–644

    Article  Google Scholar 

  12. Sakthivel S, Shankar MV, Palanichamy M, Arabindoo B, Murugesan V (2002) Photocatalytic decomposition of leather dye: comparative study of TiO2 supported on alumina and glass beads. J Photochem Photobiol, A 148:153–159

    Article  Google Scholar 

  13. Su Y, Wu Z, Wu Y, Yu J, Sun L, Lin C (2015) Acid orange II degradation through a heterogeneous Fenton-like reaction using Fe–TiO 2 nanotube arrays as a photocatalyst. J Mater Chem A 3:8537–8544

    Article  Google Scholar 

  14. Comninellis C, Kapalka A, Malato S, Parsons SA, Poulios I, Mantzavinos D (2008) Advanced oxidation processes for water treatment: advances and trends for R&D. J Chem Technol Biotechnol 83:769–776

    Article  Google Scholar 

  15. Gulkowska A, He Y, So MK, Yeung LWY, Leung HW, Giesy JP, Lam PKS, Martin M, Richardson BJ (2007) The occurrence of selected antibiotics in Hong Kong coastal waters. Mar Pollut Bull 54:1287–1306

    Article  Google Scholar 

  16. Saravanane R, Sundararaman S (2009) Effect of loading rate and HRT on the removal of cephalosporin and their intermediates during the operation of a membrane bioreactor treating pharmaceutical wastewater. Environ Technol 30:1017–1022

    Article  Google Scholar 

  17. Ajoudanian N, Nezamzadeh-Ejhieh A (2015) Enhanced photocatalytic activity of nickel oxide supported on clinoptilolite nanoparticles for the photodegradation of aqueous cephalexin. Mater Sci Semicond Process 36:162–169

    Article  Google Scholar 

  18. Kaur M, Verma A, Rajput H (2015) Potential use of foundry sand as heterogeneous catalyst in solar photo-fenton degradation of herbicide isoproturon. Int J Environ Res 9:85–92

    Google Scholar 

  19. Verma A, Prakash NT, Toor AP (2014) An efficient TiO2 coated immobilized system for the degradation studies of herbicide isoproturon: durability studies. Chemosphere 109:7–13

    Article  Google Scholar 

  20. Verma A, Prakash NT, Toor AP (2014) Photocatalytic degradation of herbicide isoproturon in TiO2 aqueous suspensions: study of reaction intermediates and degradation pathways. Environ Prog Sustain Energy 33:402–409

    Article  Google Scholar 

  21. Sheydaei M, Aber S, Khataee A (2014) Degradation of amoxicillin in aqueous solution using nanolepidocrocite chips/H2O2/UV: optimization and kinetics studies. J Ind Eng Chem 20:1772–1778

    Article  Google Scholar 

  22. Khataee A, Kasiri M, Alidokht L (2011) Application of response surface methodology in the optimization of photocatalytic removal of environmental pollutants using nanocatalysts. Environ Technol 32:1669–1684

    Article  Google Scholar 

  23. Wu J, Zhang H, Oturan N, Wang Y, Chen L, Oturan MA (2012) Application of response surface methodology to the removal of the antibiotic tetracycline by electrochemical process using carbon-felt cathode and DSA (Ti/RuO 2–IrO 2) anode. Chemosphere 87:614–620

    Article  Google Scholar 

  24. 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

    Article  Google Scholar 

  25. American Public Health Association (APHA) (1989) Standard methods for the examination of water and wastewater, 17th edn. APHA, Washington, DC

    Google Scholar 

  26. Wu T, Englehardt JD (2012) A new method for removal of hydrogen peroxide interference in the analysis of chemical oxygen demand. Environ Sci Technol 46:2291–2298

    Article  Google Scholar 

  27. Toor AP, Verma A, Singh V, Jotshi CK, Bajpai PK (2007) Photocatalytic, sonolytic and sonophotocatalytic degradation of 4-chloro-2-nitro phenol. TAPPI 6:9–13

    Google Scholar 

  28. Appavoo IA, Hu J, Huang Y, Li SFY, Ong SL (2014) Response surface modeling of Carbamazepine (CBZ) removal by Graphene-P25 nanocomposites/UVA process using central composite design. Water Res 57:270–279

    Article  Google Scholar 

  29. Rajkumar K, Muthukumar M (2012) Optimization of electro-oxidation process for the treatment of Reactive Orange 107 using response surface methodology. Environ Sci Pol Res 19:148–160

    Article  Google Scholar 

  30. Ganesh I, Kumar PP, Gupta AK, Sekhar PS, Radha K, Padmanabham G, Sundararajan G (2012) Preparation and characterization of Fe-doped TiO2 powders for solar light response and photocatalytic applications. Process App Ceramic 6:21–36

    Article  Google Scholar 

  31. Sayyar Z, Babaluo AA, Shahrouzi JR (2015) Kinetic study of formic acid degradation by Fe3+ doped TiO2 self-cleaning nanostructure surfaces prepared by cold spray. Appl Surface Sci 335:1–10

    Article  Google Scholar 

  32. Kudo A, Domen K, Maruya KI, Onishi T (1992) Reduction of nitrate ions into nitrite and ammonia over some photocatalysts. J Catal 135:300–303

    Article  Google Scholar 

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Acknowledgement

Authors would like to thank Materials Research Centre, MNIT Jaipur, India (MRC, MNITJ), and Sophisticated Analytical Instruments Laboratories, Thapar University, Patiala, India (SAI Labs), for extending their facilities for the characterization and analysis of samples.

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Correspondence to Anoop Verma.

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Bansal, P., Verma, A., Mehta, C. et al. Assessment of integrated binary process by coupling photocatalysis and photo-Fenton for the removal of cephalexin from aqueous solution. J Mater Sci 53, 7326–7343 (2018). https://doi.org/10.1007/s10853-018-2094-x

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