Abstract
Vacuum ultraviolet/ultraviolet/Fenton (VUV/UV/Fenton) is considered a novel advanced oxidation process (AOP), but little is known about its kinetics for pollutant degradation in wastewater treatment. This study systematically investigates the treatment of antibiotic-containing pharmaceutical wastewater by VUV/UV/Fenton process. A significant synergistic effect was observed during the degradation of sulfachloropyridazine (SCP, an antibiotic target) by VUV/UV/Fenton. The synergistic factor was determined to be 2.13, which means a synergistic improvement of 113% for the SCP degradation by VUV/UV/Fenton compared with the separate VUV and UV/Fenton processes. The introduction of VUV strongly accelerated the reduction of Fe3+ to Fe2+ in VUV/UV/Fenton process, which was the main reason for the synergistic effect observed. The optimal pH could be extended to near-neutral at pH 6.0 in VUV/UV/Fenton process because of the highly efficient reduction of Fe3+. A low optimal ratio of Fe2+ and H2O2 (1:25) was obtained for the VUV/UV/Fenton process, indicating a high apparent catalytic efficiency of Fe2+. Dissolved oxygen and inorganic anions such as SO42–, Cl–, HCO3– and NO3– all had various influence on the SCP degradation by VUV/UV/Fenton. TOC removal efficiency of the real pharmaceutical wastewater reached as high as 63.7% after the VUV/UV/Fenton process and meanwhile, the biodegradability index (BOD/COD) increased significantly from 0.18 to 0.46. Compared with traditional Fenton process, VUV/UV/Fenton process could save as much as 45.4% of the consumption costs for the wastewater treatment. It suggests that VUV/UV/Fenton is a promising AOP for the treatment of pharmaceutical wastewater.
Similar content being viewed by others
References
Al Hakim S, Jaber S, Zein Eddine N, Baalbaki A, Ghauch A (2020) Degradation of theophylline in a UV254/PS system: matrix effect and application to a factory effluent. Chem Eng J 380:122478. https://doi.org/10.1016/j.cej.2019.122478
Bader H, SturzeneggerHoigne VJ (1988) Photometric method for the determination of low concentrations of hydrogen peroxide by the peroxidase catalyzed oxidation of N, N-diethyl-p-phenylenediamine (DPD). Water Res 22:1109–1115. https://doi.org/10.1016/0043-1354(88)90005-X
Bolton JR, Brcher KG, Tumas W, TolMan C (2001) Figures of merit for the technical development and application of advanced oxidation technologies for both electric- and solar-driven systems. Pure App Chem 73:627–637. https://doi.org/10.1351/pac200173040627
Buchanan W, Roddick F, Porter N, Drikas M (2005) Fractionation of UV and VUV pretreated natural organic matter from drinking water. Environ Sci Technol 39:4647–4654. https://doi.org/10.1021/es048489+
Clarizia L, Russo D, Di Somma I, Marotta R, Andreozzi R (2017) Homogeneous photo-Fenton processes at near neutral pH: A review. App Catal B 209:358–371. https://doi.org/10.1016/j.apcatb.2017.03.011
Gonzalez MC, Braun AM (1995) VUV photolysis of aqueous solutions of nitrate and nitrite. Res Chem Lntermed 21:837–859. https://doi.org/10.1163/156856795X00512
Gonzalez MC, Braun AM (1996) Vacuum-UV photolysis of aqueous solutions of nitrate: effect of organic matter I Phenol. J Photochem Photobiol A 93:7–19. https://doi.org/10.1016/1010-6030(95)04127-3
Gonzalez MG, Oliveros E, Worner M, Braun AM (2004) Vacuum-ultraviolet photolysis of aqueous reaction systems. J Photochem Photobiol C 5:225–246. https://doi.org/10.1016/j.jphotochemrev.2004.10.002
Imoberdorf G, Mohseni M (2011) Degradation of natural organic matter in surface water using vacuum-UV irradiation. J Hazard Mater 186:240–246. https://doi.org/10.1016/j.jhazmat.2010.10.118
Li MK, Qiang ZM, Hou P, Bolton JR, Qu JH, Li P, Wang C (2016) VUV/UV/chlorine as an enhanced advanced oxidation process for organic pollutant removal from water: assessment with a novel mini-fluidic VUV/UV photoreaction system (MVPS). Environ Sci Technol 50:5849–5856. https://doi.org/10.1021/acs.est.6b00133
Lin YT, Wang YH, Wu JCS, Wang X (2021) Photo-Fenton enhanced twin-reactor for simultaneously hydrogen separation and organic wastewater degradation. App Catal B 281:119517. https://doi.org/10.1016/j.apcatb.2020.119517
Liu Y, Fan Q, Wang J (2018) Zn-Fe-CNTs catalytic in situ generation of H2O2 for Fenton-like degradation of sulfamethoxazole. J Hazard Mater 342:166–176. https://doi.org/10.1016/j.jhazmat.2017.08.016
Liu L, Chen Z, Zhang J, Shan D, Wu Y, Bai L, Wang B (2021) Treatment of industrial dye wastewater and pharmaceutical residue wastewater by advanced oxidation processes and its combination with nanocatalysts: a review. J Water Process Eng 42:102122. https://doi.org/10.1016/j.jwpe.2021.102122
López-Vinent N, Cruz-Alcalde A, Gutiérrez C, Marco P, Giménez J, Esplugas S (2020) Micropollutant removal in real WW by photo-Fenton (circumneutral and acid pH) with BLB and LED lamps. Chem Eng J 379:122416. https://doi.org/10.1016/j.cej.2019.122416
López-Vinent N, Cruz-Alcalde A, Giménez J, Esplugas S, Sans C (2021) Improvement of the photo-Fenton process at natural condition of pH using organic fertilizers mixtures: potential application to agricultural reuse of wastewater. App Catal B 290:120066. https://doi.org/10.1016/j.apcatb.2021.120066
Qiang ZM, Liu C, Dong BZ, Zhang YL (2010) Degradation mechanism of alachlor during direct ozonation and O3/H2O2 advanced oxidation process. Chemosphere 78:517–526. https://doi.org/10.1016/j.chemosphere.2009.11.037
Rodríguez-Narváez OM, Pérez LS, Yee NG, Peralta-Hernández JM, Bandala ER (2018) Comparison between Fenton and Fenton-like reactions for l-proline degradation. Intern J Environ Sci Technol 16:1515–1526. https://doi.org/10.1007/s13762-018-1764-1
Samy M, Ibrahim MG, Gar Alalm M, Fujii M (2020) MIL-53(Al)/ZnO coated plates with high photocatalytic activity for extended degradation of trimethoprim via novel photocatalytic reactor. Sep Purif Technol 249:117173. https://doi.org/10.1016/j.seppur.2020.117173
Thomas N, Dionysiou DD, Pillai SC (2021) Heterogeneous Fenton catalysts: a review of recent advances. J Hazard Mater 404:124082. https://doi.org/10.1016/j.jhazmat.2020.124082
Vorontsov AV (2019) Advancing Fenton and photo-Fenton water treatment through the catalyst design. J Hazard Mater 372:103–112. https://doi.org/10.1016/j.jhazmat.2018.04.033
Wang C, Zhang J, Du J, Zhang P, Zhao Z, Shi W, Cui F (2021) Rapid degradation of norfloxacin by VUV/Fe(2+)/H2O2 over a wide initial pH: process parameters, synergistic mechanism, and influencing factors. J Hazard Mater 416:125893. https://doi.org/10.1016/j.jhazmat.2021.125893
Wen D, Wu ZD, Tang YB, Li MK, Qiang ZM (2018) Accelerated degradation of sulfamethazine in water by VUV/UV photo-Fenton process: impact of sulfamethazine concentration on reaction mechanism. J Hazard Mater 344:1181–1187. https://doi.org/10.1016/j.jhazmat.2017.10.032
Xu J, Dai G, Chen B, He D, Situ Y, Huang H (2020) Construction of Ti(3+)-TiO2-C3N4por compound coupling photocatalysis and Fenton-like process: self-driven Fenton-like process without extra H2O2 addition. Chemosphere 241:125022. https://doi.org/10.1016/j.chemosphere.2019.125022
Yang L, Yao G (2022) A modified spectrophotometric method for the determination of ferrous ion during the Fenton process. Intern J Environ Anal Chem 102:3194–3206. https://doi.org/10.1080/03067319.2020.1766034
Yang LX, Zhang ZH (2019) Degradation of six typical pesticides in water by VUV/UV/chlorine process: evaluation of the synergistic effect. Water Res 161:439–447. https://doi.org/10.1016/j.watres.2019.06.021
Yang L, Zhou J, Feng Y (2022) Treatment of fluorine-containing pharmaceutical wastewater by VUV/UV process. Environ Sci Pollut Res Int 29:20289–20295. https://doi.org/10.1007/s11356-021-17063-8
Yoon J, Lee Y, Kim S (2001) Investigation of the reaction pathway of OH radicals produced by Fenton oxidation in the conditions of wastewater treatment. Water Sci Technol 44:15–21. https://doi.org/10.2166/wst.2001.0242
Zaied BK, Rashid M, Nasrullah M, Zularisam AW, Pant D, Singh L (2020) A comprehensive review on contaminants removal from pharmaceutical wastewater by electrocoagulation process. Sci Total Environ 726:138095. https://doi.org/10.1016/j.scitotenv.2020.138095
Acknowledgements
This paper was financially supported by the Natural Science Foundation of Hunan Province (Grant No. 2022JJ50227), Shaoyang University (CX2023SY041) and Education Department of Hunan Province (Grant No. 21B0687).
Author information
Authors and Affiliations
Contributions
LY contributed to visualization, investigation, reviewing and editing; FX contributed to conceptualization, original draft preparation and methodology.
Corresponding author
Ethics declarations
Conflict of interest
We declare that we do not have any commercial or associative interest that represents a conflict of interest in connection with the work titled “Treatment of antibiotic-containing pharmaceutical wastewater by the novel VUV/UV/Fenton process at near-neutral pH”.
Additional information
Editorial responsibility: Maryam Shabani.
Supplementary Information
Below is the link to the electronic supplementary material.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Yang, L., Xue, F. Treatment of antibiotic-containing pharmaceutical wastewater by the novel VUV/UV/Fenton process at near-neutral pH. Int. J. Environ. Sci. Technol. 21, 3889–3898 (2024). https://doi.org/10.1007/s13762-023-05240-w
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s13762-023-05240-w