Abstract
The recent increase in the global consumption of antibiotics has led to faster entry of these pollutants into the environment as well as an increase in public concern about its impact on ecosystem and human health. Generally, due to high toxicity of antibiotics, biological methods are not used to treat these pollutants; therefore, advanced oxidation processes are recommended to treat and reduce the toxicity of the wastewater. In this study, we evaluated the efficacy of photo-oxidation (P) and electro-oxidation (E) processes in the removal of amoxicillin (AMX) from wastewater, either as integrated or separate processes. Moreover, the effect of variables, including current density (2-100 mA/cm2), reaction time (2–120 min), and electrolyte concentration (100–1,000 mg/l) on antibiotic removal efficiency were investigated by Box Behnken design under response surface methodology, and optimal conditions were determined for pollutant removal. Then, the effect of AMX concentration and pH variables on the removal efficiency was investigated. The COD removal efficiency was also evaluated under optimal conditions, and eventually the toxicity and bioavailability of the effluent from the combined Photo-Electro oxidation process (PE) were examined. The optimal conditions for variables, including current density, reaction time, and electrolyte concentration for removal efficiency of 62.4%, were 94 mA/cm2, 95 min and 997 mg/l, respectively. Investigating the Amoxicillin and pH variables showed that by reducing the contaminant concentration and pH, the antibiotic removal efficiency increased. The toxicity and bioavailability of the final effluent show the reduction of both parameters in the PE reactor effluent. The PE process can provide an appropriate function to reduce the toxicity and antibacterial properties of effluent by removing more than 60% of amoxicillin and 30% of COD from wastewater.
Similar content being viewed by others
References
F. Sopaj, M. A. Rodrigo, N. Oturan, F. I. Podvorica, J. Pinson and M. A. Oturan, Chem. Eng. J., 262, 286 (2015).
M. Klavarioti, D. Mantzavinos and D. Kassinos, Environ. Int., 5(2), 402 (2009).
T.P. Van Boeckel, S. Gandra, A. Ashok, Q. Caudron, B. T. Grenfell, S. A. Levin and R. Laxminarayan, The Lancet Infectious Diseases., 14(8), 742 (2014).
W.-h. Xu, G. Zhang, S.-c. Zou, X.-d. Li and Y.-c. Liu, Environ. Pollut., 145(3), 672 (2007).
A. G. Trovo, R. F. P. Nogueira, A. Agüera, A. R. Fernandez-Alba and S. Malato, Water Res., 45(3), 1394 (2011).
. F. Ayand F. Kargi, J. Hazard. Mater., 179(1-3), 622 (2010).
E. S. Elmolla and M. Chaudhuri, J. Hazard. Mater., 172(2–3), 1476 (2009).
E. Commission, Off J. Eur. Union., 15, 1 (2010).
A. C. Moffat, M. D. Osselton, B. Widdop and J. Watts, Clarke’s analysis of drugs and poisons, Pharmaceutical Press London (2011).
X. Yu, J. Zuo, R. Li, L. Gan, Z. Li and F. Zhang, Ecotoxicol. Environ. Saf., 106, 40 (2014).
C. Sirtori, A. Zapata, I. Oller, W. Gernjak, A. Agüera and S. Malato, Water Res., 43(3), 661 (2009).
N. De la Cruz, J. Giménez, S. Esplugas, D. Grandjean, L. De Alencastro and C. Pulgarin, Water Res., 46(6), 1947 (2012).
I. Sirés and E. Brillas, Environ. Int., 40, 212 (2012).
A. Dirany, I. Sirés, N. Oturan, A. Özcan and M. A. Oturan, Environ. Sci. Technol., 46(7), 4074 (2012).
S. Cotillas, M. J. M. de Vidales, J. Llanos, C. Sáez, P. Canizares and M. A. Rodrigo, J. Hazard. Mater., 319, 93 (2016).
M. Taghi Ghaneian, A. Ebrahimi, J. Salimi, R. Khosravi, R. A. Fallahzadeh, M. Amrollahi and M. Taghavi, J. Mazandaran University of Medical Sci., 26(137), 159 (2016).
M. Farzadkia, Y. Dadban Shahamat, S. Nasseri, A. H. Mahvi, M. Gholami and A. Shahryari, J. Eng., 2014 (2014).
M. Panizza and G. Cerisola, J. Electroanal. Chem., 638(1), 28 (2010).
N. Oturan, E. Brillas and M. A. Oturan, Environ. Chem. Lett., 10(2), 165 (2012).
N. B. Tahar and A. Savall, Electrochim. Acta, 54(21), 4809 (2009).
E. Bazrafshan, A. Mahvi, S. Nasseri and M. Shaieghi, Iranian J. Environ. Health, Sci. Eng., 4(2), 127 (2007).
A. Dalvand, M. Gholami, A. Joneidi and N. M. Mahmoodi, CLEAN-Soil, Air, Water, 39(7), 665 (2011).
J. Nouri, A. Mahvi and E. Bazrafshan, Int. J. Environ. Res., 4(2), 201 (2010).
M. Alimohammadi, M. Askari, M. Dehghani, A. Dalvand, R. Saeedi, K. Yetilmezsoy, B. Heibati and G. McKay, Int. J. Environ. Sci. Technol., 14(10), 2125 (2017).
N. M. Mahmoodi and A. Dalvand, Desalination Water Treatment., 51(31–33), 5959 (2013).
L. Shan, J. Liu, J. J. Ambuchi, Y. Yu, L. Huang and Y. Feng, Chem. Eng. J., 323, 455 (2017).
M. Taghavi, M. T. Ghaneian, M. H. Ehrampoush, M. Tabatabaee, M. Afsharnia, A. Alami and J. Mardaneh, Environ. Monit. Assess., 190(4), 188 (2018).
G. Safari, M. Hoseini, M. Seyedsalehi, H. Kamani, J. Jaafari and A. Mahvi, Int. J. Environ. Sci. Technol., 12(2), 603 (2015).
A. Dalvand, M. Khoobi, R. Nabizadeh, M. R. Ganjali, E. Gholibegloo and A. H. Mahvi, J. Poly m. Environ., 26(8), 3470 (2018).
A. D. Eaton, L. S. Clesceri, A. E. Greenberg and M. A. H. Franson, Am. Public Health Assoc., 1015, 49 (2005).
E. A. Serna-Galvis, K. E. Berrio-Perlaza and R. A. Torres-Palma, Environ. Sci. Pollut. Res., 24(30), 23771 (2017).
L. Szabó, T. Tóth, T. Engelhardt, G. Rácz, C. Mohácsi-Farkas, E. Takács and L. Wojnárovits, Sci. Total Environ., 551, 393 (2016).
D. Hosiner, S. Gerber, H. Lichtenberg-Frate, W. Glaser, C. Schüller and E. Klipp, PLoS One, 9(1), e83330 (2014).
F. C. Moreira, R. A. Boaventura, E. Brillas and V. J. Vilar, Appl. Catal. B: Environ., 202, 217 (2017).
B. Boye, M. M. Dieng and E. Brillas, Environ. Sci. Technol., 36(13), 3030 (2002).
A. Serra, X. Domenech, C. Arias, E. Brillas and J. Peral, Appl. Catal. B: Environ., 89(1–2), 12 (2009).
A. Fernandes, M. Pacheco, L. Ciríaco and A. Lopes, J. Haz ard. Mater., 199, 82 (2012).
V. S. Antonin, S. Garcia-Segura, M. C. Santos and E. Brillas, J. Electroanal. Chem., 747, 1 (2015).
V. Orescanin, R. Kollar, K. Nad, I. L. Mikelic and S. F. Gustek, J. Environ. Sci. Health, Part A., 48(12), 1543 (2013).
A. Thiam, M. Zhou, E. Brillas and I. Sirés, Appl. Catal. B: Environ., 150, 116 (2014).
C. Carvalho, A. Fernandes, A. Lopes, H. Pinheiro and I. Gonçalves, Chemosphere, 67(7), 1316 (2007).
A. Thiam, I. Sirés, J. A. Garrido, R. M. Rodríguez and E. Brillas, J. Hazard. Mater., 290, 34 (2015).
M. Panizza and G. Cerisola, Chem. Rev., 109(12), 6541 (2009).
A. Sánchez-Carretero, C. Sáez, P. Cañizares and M. Rodrigo, Chem. Eng. J., 166(2), 710 (2011).
C. Flox, J. A. Garrido, R. M. Rodríguez, P.-L. Cabot, F. Centellas, C. Arias and E. Brillas, Catal. Today, 129(1–2), 29 (2007).
S. Hammami, N. Oturan, N. Bellakhal, M. Dachraoui and M. A. Oturan, J. Electroanal. Chem., 610(1), 75 (2007).
E. Isarain-Chávez, R. M. Rodríguez, J. A. Garrido, C. Arias, F. Centellas, P. L. Cabot and E. Brillas, Electrochim. Acta, 56(1), 215 (2010).
A. El-Ghenymy, R. M. Rodríguez, C. Arias, F. Centellas, J. A. Garrido, P. L. Cabot and E. Brillas, J. Electroanal. Chem., 701, 7 (2013).
L. Labiadh, M. A. Oturan, M. Panizza, N. B. Hamadi and S. Ammar, J. Hazard. Mater., 297, 34 (2015).
M. Iranifam, M. Zarei and A. Khataee, J. Electroanal. Chem., 659(1), 107 (2011).
J. Wu, H. Zhang, N. Oturan, Y. Wang, L. Chen and M. A. Oturan, Chemosphere, 87(6), 614 (2012).
A. Khataee, H. Marandizadeh, M. Zarei, S. Aber, B. Vahid, Y. Hanifehpour and S. W. Joo, Curr. Nanoscience., 9(3), 387 (2013).
A. H. Mahvi, S. J. A.-d. Ebrahimi, A. Mesdaghinia, H. Gharibi and M. H. Sowlat, J. Hazard. Mater., 192(3), 1267 (2011).
H. T. Madsen, E. G. Søgaard and J. Muff, Chem. Eng. J., 276, 358 (2015).
A. Zuorro, M. Fidaleo and R. Lavecchia, J. Environ. Manage., 127, 28 (2013).
F. Chen, S. Xie, X. Huang and X. Qiu, J. Hazard. Mater., 322, 152 (2017).
F. Hine, Electrode processes and electrochemical engineering, Springer Science & Business Media (2012).
E. Brillas and C. A. Martínez-Huitle, Appl. Catal. B: Environ., 166, 603 (2015).
A. K. Abdessalem, M. A. Oturan, N. Oturan, N. Bellakhal and M. Dachraoui, Int. J. Environ. Anal. Chem., 90(3–6), 468 (2010).
S. Garcia-Segura, J. Keller, E. Brillas and J. Radjenovic, J. Haz ard. Mater., 283, 551 (2015).
A. El-Ghenymy, N. Oturan, M. A. Oturan, J. A. Garrido, P. L. Cabot, F. Centellas, R. M. Rodríguez and E. Brillas, Chem. Eng. J., 234, 115 (2013).
F.C. Moreira, J. Soler, A. Fonseca, I. Saraiva, R. A. Boaventura, E. Brillas and V. J. Vilar, Appl. Catal. B: Environ., 182, 161 (2016).
G. V. Buxton, C. L. Greenstock, W. P. Helman and A. B. Ross, J. Phys. Chem. Reference Data, 17(2), 513 (1988).
C. Flox, S. Ammar, C. Arias, E. Brillas, A. V. Vargas-Zavala and R. Abdelhedi, Appl. Catal. B: Environ., 67(1–2), 93 (2006).
Y. Fan, Z. Ai and L. Zhang, J. Hazard. Mater., 176(1–3), 678 (2010).
R. Salazar, S. Garcia-Segura, M. Ureta-Zañartu and E. Brillas, Electrochim. Acta, 56(18), 6371 (2011).
E. Guinea, C. Arias, P. L. Cabot, J. A. Garrido, R. M. Rodríguez, F. Centellas and E. Brillas, Water Res., 42(1–2), 499 (2008).
A. M. de Freitas, C. Sirtori and P. Peralta-Zamora, Environ. Chem. Lett., 9(1), 97 (2011).
E. Bazrafshan, A. H. Mahvi, S. Naseri and A. R. Mesdaghinia, Turkish J. Eng. Environ. Sci., 32(2), 59 (2008).
S. Cotillas, J. Llanos, O. G. Miranda, G. C. Díaz-Trujillo, P. Cañiza-res and M. A. Rodrigo, Electrochim. Acta, 140, 396 (2014).
M. T. Ghaneian, M. Tabatabaee, M. H. Ehrampoush, A. Jebali, S. Hekmatimoghaddam, H. Fallahzadeh and R. A. Fallahzadeh, Pharm. Chem. J., 49(3), 210 (2015).
Acknowledgement
We appreciate the technical support from the Environmental Science and Technology research center at Shahid Sadoughi University of Medical Sciences in Yazd, Iran.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Fallahzadeh, R.A., Mahvi, A.H., Meybodi, M.N. et al. Application of photo-electro oxidation process for amoxicillin removal from aqueous solution: Modeling and toxicity evaluation. Korean J. Chem. Eng. 36, 713–721 (2019). https://doi.org/10.1007/s11814-019-0259-1
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11814-019-0259-1