Abstract
A comparative study on the mineralization of antibiotic trimethoprim (TMP) in neutral medium was investigated by applying irradiation with five types of ultraviolet lamps. Among these lamps, the whole envelope of one lamp contained ordinary quartz, which could only transmit ultraviolet-C (UVC) light. For the other four lamps, approximately one tenth, a quarter, a half, and full of envelopes were comprised of high-purity synthetic quartz, which can transmit both vacuum ultraviolet (VUV) and UVC light. TMP decay was well fitted to pseudo-first-order reaction kinetics and occurred more quickly as the VUV intensity increased. Poor mineralization was achieved in the absence of VUV light, whereas the mineralization efficiency was also enhanced with increasing VUV intensity. The presence of hydroxyl radicals (•OH), superoxide radicals (O2•−) and singlet oxygen (1O2) during VUV photolysis of water was confirmed by electron paramagnetic resonance (EPR) analysis. Appropriate radical quenching experiments and fluorescent molecular probe detection provided the evidence that •OH played a significant role in TMP mineralization. Higher VUV intensity favored the generation of H2O2 and •OH. The evolution of NH4+ and NO3− as well as carboxylic acids (formic, acetic, oxalic, and oxamic acids) released in the treated solution were quantified. Ten aromatic intermediates were also identified by UPLC-QTOF-MS. Thereby, a plausible reaction sequence for TMP mineralization in VUV/UVC photolysis was finally proposed.
Graphical Abstract
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
Data availability
The data sets used or analyzed in the current study are available from the corresponding author upon reasonable request.
References
Ali I, Kon’kova T, Kasianov V, Rysev A, Panglisch S, Mbianda XY, Habila MA, AlMasoud N (2021) Preparation and characterization of nano-structured modified montmorillonite for dioxidine antibacterial drug removal in water. J Mol Liq 331:115770. https://doi.org/10.1016/j.molliq.2021.115770
Azrague K, Bonnefille E, Pradines V, Pimienta V, Oliveros E, Maurette MT, Benoit-Marquie F (2005) Hydrogen peroxide evolution during VUV photolysis of water. Photochem Photobiol Sci 4(5):406–408. https://doi.org/10.1039/b500162e
Bagheri M, Mohseni M (2015) A study of enhanced performance of VUV/UV process for the degradation of micropollutants from contaminated water. J Hazard Mater 294:1–8. https://doi.org/10.1016/j.jhazmat.2015.03.036
Bengtsson-Palme J, Hammaren R, Pal C, Ostman M, Bjorlenius B, Flach CF, Fick J, Kristiansson E, Tysklind M, Larsson DGJ (2016) Elucidating selection processes for antibiotic resistance in sewage treatment plants using metagenomics. Sci Total Environ 572:697–712. https://doi.org/10.1016/j.scitotenv.2016.06.228
Borras N, Arias C, Oliver R, Brillas E (2011) Mineralization of desmetryne by electrochemical advanced oxidation processes using a boron-doped diamond anode and an oxygen-diffusion cathode. Chemosphere 85(7):1167–1175. https://doi.org/10.1016/j.chemosphere.2011.09.008
Chen Y, Ye J, Chen Y, Hu H, Zhang H, Ou H (2019) Degradation kinetics, mechanism and toxicology of tris(2-chloroethyl) phosphate with 185 nm vacuum ultraviolet. Chem Eng J 356:98–106. https://doi.org/10.1016/j.cej.2018.09.007
Czili H, Horváth A (2008) Applicability of coumarin for detecting and measuring hydroxyl radicals generated by photoexcitation of TiO2 nanoparticles. Appl Catal b: Environ 81(3–4):295–302. https://doi.org/10.1016/j.apcatb.2008.01.001
Fatta-Kassinos D, Meric S, Nikolaou A (2011) Pharmaceutical residues in environmental waters and wastewater: current state of knowledge and future research. Anal Bioanal Chem 399(1):251–275. https://doi.org/10.1007/s00216-010-43009
Garza-Campos BR, Guzman-Mar JL, Reyes LH, Brillas E, Hernandez-Ramirez A, Ruiz-Ruiz EJ (2014) Coupling of solar photoelectro-Fenton with a BDD anode and solar heterogeneous photocatalysis for the mineralization of the herbicide atrazine. Chemosphere 97:26–33. https://doi.org/10.1016/j.chemosphere.2013.10.044
Ge L, Chen J, Wei X, Zhang S, Qiao X, Cai X, Xie Q (2018) Aquatic photochemistry of fluoroquinolone antibiotics: kinetics, pathways, and multivariate effects of main water constituents. Environ Sci Technol 44:2400–2405. https://doi.org/10.1021/es902852v
Geng C, Liang Z, Cui F, Zhao Z, Yuan C, Du J, Wang C (2020) Energy-saving photo-degradation of three fluoroquinolone antibiotics under VUV/UV irradiation: Kinetics, mechanism, and antibacterial activity reduction. Chem Eng J 383:123145. https://doi.org/10.1016/j.cej.2019.123145
Gonçalves NPF, del Puerto O, Medana C, Calza P, Roslev P (2021) Degradation of the antifungal pharmaceutical clotrimazole by UVC and vacuum-UV irradiation: Kinetics, transformation products and attenuation of toxicity. J Environ Chem Eng 9(5):106275. https://doi.org/10.1016/j.jece.2021.106275
Gonzalez M, Oliveros E, Worner M, Braun AM (2004) Vacuum-ultraviolet photolysis of aqueous reaction systems. J Photochem Photobiol C: Photochem Rev 5(3):225–246. https://doi.org/10.1016/j.jphoto-chemrev.2004.10.002
Han S, Wang Z, Huang H, Wang T, Zhou Z, Bai Y, Du P, Li X (2022) Estimating antibiotics use in major cities in China through wastewater-based epidemiology. Sci Total Environ 826:154116
Hancu G, Sasebesi A, Rusu A, Kelemen H, Ciurba A (2015) Study of the electrophoretic behavior of cephalosporins by capillary zone electrophoresis. Adv Pharm Bull 5(2):223–9. https://doi.org/10.15171/apb.2015.031
Hassani A, Krishnan S, Scaria J, Eghbali P, Nidheesh PV (2021) Z-scheme photocatalysts for visible-light-driven pollutants degradation: A review on recent advancements. Curr Opin Solid ST m 25:100941. https://doi.org/10.1016/j.cossms.2021.100941
Hassani A, Eghbali P, Mahdipour F, Wacławek S, Lin K-YA, Ghanbari F (2023) Insights into the synergistic role of photocatalytic activation of peroxymonosulfate by UVA-LED irradiation over CoFe2O4-rGO nanocomposite towards effective Bisphenol A degradation: Performance, mineralization, and activation mechanism. Chem Eng J 453:139556. https://doi.org/10.1016/j.cej.2022.139556
Heit G, Braun AM (1997) VUV-Photolysis of aqueouos systems: spatial differentiation between volumes of primary and secondary reactions. Water Sci Technol 35(4):25–30. https://doi.org/10.1016/S0273-1223(97)00005-X
Huang L, Jing H, Cheng Z, Dong W (2013) Different photodegradation behavior of 4-tert-octylphenol under UV and VUV irradiation in aqueous solution. J Photoch Photobio a 251:69–77. https://doi.org/10.1016/j.jphotochem.2012.10.014
Ji Y, Xie W, Fan Y, Shi Y, Kong D, Lu J (2016) Degradation of trimethoprim by thermo-activated persulfate oxidation: Reaction kinetics and transformation mechanisms. Chem Eng J 286:16–24. https://doi.org/10.1016/j.cej.2015.10.050
Jiang F, Qiu B, Sun D (2018) Advanced degradation of refractory pollutants in incineration leachate by UV/Peroxymonosulfate. Chem Eng J 349:338–346. https://doi.org/10.1016/j.cej.2018.05.062
Karimian S, Moussavi G, Fanaei F, Mohammadi S, Shekoohiyan S, Giannakis S (2020) Shedding light on the catalytic synergies between Fe(II) and PMS in vacuum UV (VUV/Fe/PMS) photoreactors for accelerated elimination of pharmaceuticals: The case of metformin. Chem Eng J 400:125896. https://doi.org/10.1016/j.cej.2020.125896
Kuang J, Huang J, Wang B, Cao Q, Deng S, Yu G (2013) Ozonation of trimethoprim in aqueous solution: identification of reaction products and their toxicity. Water Res 47(8):2863–2872. https://doi.org/10.1016/j.watres.2013.02.048
Li M, Wang C, Yau M, Bolton JR, Qiang Z (2017) Sulfamethazine degradation in water by the VUV/UV process: Kinetics, mechanism and antibacterial activity determination based on a mini-fluidic VUV/UV photoreaction system. Water Res 108:348–355. https://doi.org/10.1016/j.watres.2016.11.018
Liang C, Zhao H, Deng M, Quan X, Chen S, Wang H (2015) Impact of dissolved organic matter on the photolysis of the ionizable antibiotic norfloxacin. J Environ Sci (china) 27:115–123. https://doi.org/10.1016/j.jes.2014.08.015
Liu X, Zhang X, Shao K, Lin C, Li C, Ge F, Dong Y (2016) Fe0-activated persulfate-assisted mechanochemical destruction of expired compound sulfamethoxazole tablets. RSC Adv 6(25):20938–20948. https://doi.org/10.1039/c5ra27113d
Liu C, Liu S, Liu L, Tian X, Liu L, Xia Y, Liang X, Wang Y, Song Z, Zhang Y, Li R, Liu Y, Qi F, Ikhlaq A (2020) Novel Carbon-based Fe-Co Oxides Derived from Prussian Blue Analogues Activating Peroxymonosulfate: Refractory Drugs Degradation without Metal Leaching. Chem Eng J 379:122274. https://doi.org/10.1016/j.cej.2019.122274
Liu G, Feng M, Tayyab M, Gong J, Zhang M, Yang M, Lin K (2021a) Direct and efficient reduction of perfluorooctanoic acid using bimetallic catalyst supported on carbon. J Hazard Mater 412:125224. https://doi.org/10.1016/j.jhazmat.2021.125224
Liu Y, Zhu Q, Tayyab M, Zhou L, Lei J, Zhang J (2021b) Single-Atom Pt Loaded Zinc Vacancies ZnO–ZnS Induced Type-V Electron Transport for Efficiency Photocatalytic H2 Evolution. Sol Rrl 5:2100536. https://doi.org/10.1002/solr.202100536
Luo X, Zheng Z, Greaves J, Cooper WJ, Song W (2012) Trimethoprim: kinetic and mechanistic considerations in photochemical environmental fate and AOP treatment. Water Res 46(4):1327–1336. https://doi.org/10.1016/j.watres.2011.12.052
Masjoudi M, Mohseni M (2023) Photolysis of chloramines in vacuum-UV and vacuum-UV/chlorine advanced oxidation processes for removal of 1,4-dioxane: Effect of water matrix, kinetic modeling, and implications for potable reuse. J Hazard Mater 454:131454. https://doi.org/10.1016/j.jhazmat.2023.131454
Michael I, Hapeshi E, Osorio V, Perez S, Petrovic M, Zapata A, Malato S, Barcelo D, Fatta-Kassinos D (2012) Solar photocatalytic treatment of trimethoprim in four environmental matrices at a pilot scale: transformation products and ecotoxicity evaluation. Sci Total Environ 430:167–173. https://doi.org/10.1016/j.scitotenv.2012.05.003
Moussavi G, Mahdavianpour M (2016) The selective direct oxidation of ammonium in the contaminated water to nitrogen gas using the chemical-less VUV photochemical continuous-flow reactor. Chem Eng J 295:57–63. https://doi.org/10.1016/j.cej.2016.03.035
Moussavi G, Rezaei M, Pourakbar M (2018) Comparing VUV and VUV/Fe2+ processes for decomposition of cloxacillin antibiotic: Degradation rate and pathways, mineralization and by-product analysis. Chem Eng J 332:140–149. https://doi.org/10.1016/j.cej.2017.09.057
Náfrádi M, Farkas L, Alapi T, Hernádi K, Kovács K, Wojnárovits L, Takács E (2020) Application of coumarin and coumarin-3-carboxylic acid for the determination of hydroxyl radicals during different advanced oxidation processes. Radiat Phys Chem 170:108610. https://doi.org/10.1016/j.radphyschem.2019.108610
Nosaka Y, Nosaka AY (2017) Generation and detection of reactive oxygen species in photocatalysis. Chem Rev 117(17):11302–11336. https://doi.org/10.1021/acs.chemrev.7b00161
Ohguri N, Nosaka AY, Nosaka Y (2010) Detection of •OH radicals as the effect of Pt particles in the membrane of polymer electrolyte fuel cells. J Power Sources 195(15):4647–4652. https://doi.org/10.1016/j.jpowsour.2010.02.010
Paula FC, Pietro AC, Cass QB (2008) Simultaneous quantification of sulfamethoxazole and trimethoprim in whole egg samples by column-switching high-performance liquid chromatography using restricted access media column for on-line sample clean-up. J Chromatogr A 1189(1–2):221–226. https://doi.org/10.1016/j.chroma.2007.08.046
Rafqah S, Wong-Wah-Chung P, Aamili A, Sarakha M (2005) Degradation of metsulfuron methyl by heterogeneous photocatalysis on TiO2 in aqueous suspensions: Kinetic and analytical studies. J Mol Catal a: Chem 237(1–2):50–59. https://doi.org/10.1016/j.molcata.2005.03.044
Robl S, Worner M, Maier D, Braun AM (2012) Formation of hydrogen peroxide by VUV-photolysis of water and aqueous solutions with methanol. Photochem Photobiol Sci 11(6):1041–1050. https://doi.org/10.1039/c2pp05381k
Rosal R, Rodríguez A, Gonzalo MS, García-Calvo E (2008) Catalytic ozonation of naproxen and carbamazepine on titanium dioxide. Appl Catal b: Environ 84(1–2):48–57. https://doi.org/10.1016/j.apcatb.2008.03.003
Serna-Galvis EA, Ferraro F, Silva-Agredo J, Torres-Palma RA (2017) Degradation of highly consumed fluoroquinolones, penicillins and cephalosporins in distilled water and simulated hospital wastewater by UV254 and UV254/persulfate processes. Water Res 122:128–138. https://doi.org/10.1016/j.watres.2017.05.065
Sirtori C, Aguera A, Gernjak W, Malato S (2010) Effect of water-matrix composition on Trimethoprim solar photodegradation kinetics and pathways. Water Res 44(9):2735–2744. https://doi.org/10.1016/j.watres.2010.02.006
Sopaj F, Oturan N, Pinson J, Podvorica F, Oturan MA (2016) Effect of the anode materials on the efficiency of the electro-Fenton process for the mineralization of the antibiotic sulfamethazine. Appl Catal b: Environ 199:331–341. https://doi.org/10.1016/j.apcatb.2016.06.035
Spulber M, Schlick S (2010) Using cyclodextrins to encapsulate oxygen-centered and carbon-centered radical adducts: the case of DMPO, PBN, and MNP spin traps. J Phys Chem A 114(21):6217–6225. https://doi.org/10.1021/jp100777u
Tayyab M, Liu Y, Liu Z, Pan L, Xu Z, Yue W, Zhou L, Lei J, Zhang J (2022a) One-pot in-situ hydrothermal synthesis of ternary In2S3/Nb2O5/Nb2C Schottky/S-scheme integrated heterojunction for efficient photocatalytic hydrogen production. Curr Opin Solid ST m 628:500–512. https://doi.org/10.1016/j.jcis.2022.08.071
Tayyab M, Liu Y, Liu Z, Xu Z, Yue W, Zhou L, Lei J, Zhang J (2022b) A new breakthrough in photocatalytic hydrogen evolution by amorphous and chalcogenide enriched cocatalysts. Chem Eng J 455:140601. https://doi.org/10.1016/j.cej.2022.140601
Tayyab M, Liu Y, Min S, Irfan M, Zhu Q, Zhou L, Lei J, Zhang J (2022c) Simultaneous hydrogen production with the selective oxidation of benzyl alcohol to benzaldehyde by a noble-metal-free photocatalyst VC/CdS nanowires. Chinese J Catal 43:1165–1175. https://doi.org/10.1016/S1872-2067(21)639979
Tayyab M, Liu Y, Xu Z, Aman S, Yue W, Irfan RM, Zhou L, Zhang J (2023) Integration of redox cocatalysts for photocatalytic hydrogen evolution. In: UV‐visible photocatalysis for clean energy production and pollution remediation, pp 93-107. https://doi.org/10.1002/9783527837991.ch7
Valsania MC, Fasano F, Richardson SD, Vincenti M (2012) Investigation of the degradation of cresols in the treatments with ozone. Water Res 46(8):2795–2804. https://doi.org/10.1016/j.watres.2012.02.040
Van Boeckel TP, Gandra S, Ashok A, Caudron Q, Grenfell BT, Levin SA, Laxminarayan R (2014) Global antibiotic consumption 2000 to 2010: an analysis of national pharmaceutical sales data. Lancet Infect Dis 14(8):742–750. https://doi.org/10.1016/s1473-3099(14)70780-7
Wang B, Liu W, Zhang Y, Wang A (2020) Bioenergy recovery from wastewater accelerated by solar power: Intermittent electro-driving regulation and capacitive storage in biomass. Water Res 175:115696. https://doi.org/10.1016/j.watres.2020.115696
Wen Z, Wang A, Zhang Y, Ren S, Tian X, Li J (2019) Mineralization of cefoperazone in acid medium by the microwave discharge electrodeless lamp irradiated photoelectro-Fenton using a RuO2/Ti or boron-doped diamond anode. J Hazard Mater 374:186–194. https://doi.org/10.1016/j.jhazmat.2019.03.124
Wu Z, Yang L, Tang Y, Qiang Z, Li M (2021) Dimethoate degradation by VUV/UV process: Kinetics, mechanism and economic feasibility. Chemosphere 273:129724. https://doi.org/10.1016/j.chemosphere.2021.129724
Xiang Q, Yu J, Wong PK (2011) Quantitative characterization of hydroxyl radicals produced by various photocatalysts. J Colloid Interf Sci 357(1):163–167. https://doi.org/10.1016/j.jcis.2011.01.093
Xie P, Yue S, Ding J, Wan Y, Li X, Ma J, Wang Z (2018) Degradation of organic pollutants by Vacuum-Ultraviolet (VUV): Kinetic model and efficiency. Water Res 133:69–78. https://doi.org/10.1016/j.watres.2018.01.019
Yaghoot-Nezhad A, Wacławek S, Madihi-Bidgoli S, Hassani A, Lin K-YA, Ghanbari F (2023) Heterogeneous photocatalytic activation of electrogenerated chlorine for the production of reactive oxygen and chlorine species: A new approach for Bisphenol A degradation in saline wastewater. J Hazard Mater 445:130626. https://doi.org/10.1016/j.jhazmat.2022.130626
Yuval A, Eran F, Janin W, Oliver O, Yael D (2017) Photodegradation of micropollutants using VUV/UVC processes; Triclosan as a model compound. Sci Total Environ 601–602:397–404. https://doi.org/10.1016/j.scitotenv.2017.05.172
Zhang Y, Wang A, Tian X, Wen Z, Lv H, Li D, Li J (2016) Efficient mineralization of the antibiotic trimethoprim by solar assisted photoelectro-Fenton process driven by a photovoltaic cell. J Hazard Mater 318:319–328. https://doi.org/10.1016/j.jhazmat.2016.07.021
Zhang Q, Wang L, Chen B, Chen Y, Ma J (2020) Understanding and modeling the formation and transformation of hydrogen peroxide in water irradiated by 254 nm ultraviolet (UV) and 185 nm vacuum UV (VUV): Effects of pH and oxygen. Chemosphere 244:125483. https://doi.org/10.1016/j.chemosphere.2019.125483
Zoschke K, Bornick H, Worch E (2014) Vacuum-UV radiation at 185 nm in water treatment–a review. Water Res 52:131–145. https://doi.org/10.1016/j.watres.2013.12.034
Funding
The authors gratefully acknowledge the financial support of this work by the Fundamental Research Funds for the Central Universities (No. 2022JBZY034) and National Natural Science Foundation of China (Nos. 51978036, 51478029, 51438011).
Author information
Authors and Affiliations
Contributions
Wen Lu: Investigation; Validation; Data Curation; Formal analysis; Writing—Original Draft
Songyu Ren: Methodology; Writing—Review & Editing
Yanyu Zhang: Conceptualization; Methodology; Writing—Review & Editing
Ximeng Wen: Investigation; Validation
Zhongguo Zhang: Writing—Review & Editing
Aimin Wang: Conceptualization; Methodology; Writing—Review & Editing; Supervision
Corresponding author
Ethics declarations
Ethics approval and consents to participate
Not Applicable.
Consent for publication
The manuscript is approved by all authors for publications.
Conflict of interest
The author declare no competing interests.
Additional information
Responsible Editor: Sami Rtimi
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Highlights
• UV lamps with different VUV intensities were applied to photodegrade TMP;
• The existence of •OH, O2•-, and 1O2 in the VUV system was demonstrated;
• The role of the photogenerated H2O2 and •OH in TMP degradation was investigated;
• A comprehensive TMP degradation pathway during VUV photolysis was proposed.
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
Lu, W., Ren, S., Zhang, Y. et al. Impact of vacuum ultraviolet (VUV) intensity on the performance of VUV irradiation for the mineralization of trimethoprim in neutral media: Kinetics, mechanisms, and by-products formation. Environ Sci Pollut Res 30, 120590–120604 (2023). https://doi.org/10.1007/s11356-023-30612-7
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-023-30612-7