Alternate disinfection approaches or raise disinfectant dosages for sewage treatment plants to address the COVID-19 pandemic? From disinfection efficiency, DBP formation, and toxicity perspectives

Highlights

● Combined proposals achieved higher disinfection efficiencies than singular ones.

● Cl₂ produced the most DBPs, combined proposals can reduce their formation.

● Cl₂ could damage bacterial cell membrane and caused the leakage of IOM.

● The toxicity by zebrafish embryo followed: Cl₂≈O₃/Cl₂ > O₃ > O₃/UV/Cl₂ > UV > UV/Cl₂.

● UV/Cl₂ was suggested to deal with COVID-19 epidemic for sewage treatment plants.

Abstract

During the COVID-19 pandemic, most sewage treatment plants increased disinfectant dosages to inactivate pathogenic viruses and microorganisms more effectively. However, this approach also led to the production of more disinfection by-products (DBPs). To ensure both disinfection efficiency and a reduction in DBP formation, new disinfection protocols are required. In this study, the disinfection efficiency, DBP amounts, and toxicity changes resulting from ozone (O₃), ultraviolet (UV), chlorine (Cl₂), and their combined processes were examined. The results demonstrated that the O₃/UV/Cl₂ combination achieved the highest disinfection efficiency. Chlorination produced the most DBPs, whereas UV treatment reduced the formation of trihalomethane (THM), halogenated ketones (HKs), haloacetic acids (HAA), dichloroacetonitrile (DCAN) and N-nitrosodimethylamine (NDMA) by 45.9%, 52.6%, 82.0%, 67.95%, and 47%, respectively. O₃ also significantly reduced their production by 99.1%, 91.1%, 99.5%, 100%, and 35%. Intracellular organic matter (IOM) was identified as the primary DBP precursors, producing 2.94 times more DBPs than extracellular organic matter (EOM). The increased DBP formation during chlorination was attributed to IOM leakage and cell membrane damage, which was verified using scanning electron microscopy (SEM). The toxicities of DBPs were evaluated for six disinfection methods, revealing inconsistent results. The overall toxicities were assessed using zebrafish embryo experiments. Both evaluations indicated that chlorination alone was the least favorable method. In addition, the toxicities followed a sequence: Cl₂ ≈ O₃/Cl₂ > O₃ > O₃/UV/Cl₂ > UV > UV/Cl₂. These findings can serve as a reference for sewage treatment plants in selecting appropriate disinfection methods to manage the COVID-19 epidemic from comprehensive perspective.

Graphical abstract

Keywords

Sewage bacteria / Disinfection by-products / Toxicity / Ozonation / UV / Chlorination

References

[1] Abokifa A A, Yang Y J, Lo C S, Biswas P. (2016). Investigating the role of biofilms in trihalomethane formation in water distribution systems with a multicomponent model. Water Research, 104: 208–219

[2] APHA, AWWA, WEF (2012). Standard Methods for the Examination of Water and Wastewater. 22nd. Washington, DC: American Public Health Association/American Water Works Association/Water Environment Federation

[3] Aziz M T, Granger C O, Westerman D C, Putnam S P, Ferry J L, Richardson S D. (2022). Microseira wollei and Phormidium algae more than doubles DBP concentrations and calculated toxicity in drinking water. Water Research, 216: 118316

[4] Bei E, Li X, Wu F H, Li S X, He X S, Wang Y F, Qiu Y, Wang Y, Wang C K, Wang J. . (2020). Formation of N-nitrosodimethylamine precursors through the microbiological metabolism of nitrogenous substrates in water. Water Research, 183: 116055

[5] Beitz T, Bechmann W, Mitzner R. (1998). Investigations of reactions of selected azaarenes with radicals in water. 2. Chlorine and bromine radicals. The Journal of Physical Chemistry. A, Molecules, spectroscopy, Kinetics, Environment, & General Theory, 102(34): 6766–6771

[6] Black V J, Stewart C A, Roberts J A, Black C R. (2010). Direct effects of ozone on reproductive development in Plantago major L. populations differing in sensitivity. Environmental and Experimental Botany, 69(2): 121–128

[7] Cai G Q, Liu T Z, Zhang J S, Song H R, Jiang Q J, Zhou C. (2022). Control for chlorine resistant spore forming bacteria by the coupling of pre-oxidation and coagulation sedimentation, and UV-AOPs enhanced inactivation in drinking water treatment. Water Research, 219: 118540

[8] CDPH (2013). NDMA and Other Nitrosamines Drinking Water Issues. Sacramento, CA: California Department of Public Health

[9] Chen W, Westerhoff P, Leenheer J A, Booksh K. (2003). Fluorescence excitation−emission matrix regional integration to quantify spectra for dissolved organic matter. Environmental Science & Technology, 37(24): 5701–5710

[10] Chen X W, Chen Z, Liu H, Huang N, Mao Y, Cao K F, Shi Q, Lu Y, Hu H Y. (2022). Synergistic effects of UV and chlorine in bacterial inactivation for sustainable water reclamation and reuse. Science of the Total Environment, 845: 157320

[11] Chen Y Q, Bai F, Li Z Y, Xie P C, Wang Z P, Feng X N, Liu Z Z, Huang L Z. (2020). UV-assisted chlorination of algae-laden water: Cell lysis and disinfection byproducts formation. Chemical Engineering Journal, 383: 123165

[12] Ding X L, Zhu J Y, Zhang J, Dong T Y, Xia Y K, Jiao J D, Wang X R, Zhou W J. (2020). Developmental toxicity of disinfection by-product monohaloacetamides in embryo-larval stage of zebrafish. Ecotoxicology and Environmental Safety, 189: 110037

[13] Dong F L, Lin Q F, Li C, Wang L P, García A. (2021). UV/chlorination process of algal-laden water: algal inactivation and disinfection byproducts attenuation. Separation and Purification Technology, 257: 117896

[14] Duan X C, Liao X B, Chen J, Xie S G, Qi H, Li F, Yuan B L. (2020). THMs, HAAs and NAs production from culturable microorganisms in pipeline network by ozonation, chlorination, chloramination and joint disinfection strategies. Science of the Total Environment, 744: 140833

[15] Fang J Y, Fu Y, Shang C. (2014). The roles of reactive species in micropollutant degradation in the UV/free chlorine system. Environmental Science & Technology, 48(3): 1859–1868

[16] Gao Z C, Lin Y L, Xu B, Xia Y, Hu C Y, Zhang T Y, Qian H, Cao T C, Gao N Y. (2020). Effect of bromide and iodide on halogenated by-product formation from different organic precursors during UV/chlorine processes. Water Research, 182: 116035

[17] Gorito A M, Ribeiro A R L, Rodrigues P, Pereira M F R, Guimarães L, Almeida C M R, Silva A M T. (2022). Antibiotics removal from aquaculture effluents by ozonation: chemical and toxicity descriptors. Water Research, 218: 118497

[18] Guo K H, Wu Z H, Shang C, Yao B, Hou S D, Yang X, Song W H, Fang J Y. (2017). Radical chemistry and structural relationships of PPCP degradation by UV/chlorine treatment in simulated drinking water. Environmental Science & Technology, 51(18): 10431–10439

[19] Guo M T, Huang J J, Hu H Y, Liu W J. (2011). Growth and repair potential of three species of bacteria in reclaimed wastewater after UV disinfection. Biomedical and Environmental Sciences, 24(4): 400–407

[20] Hijnen W A M, Beerendonk E F, Medema G J. (2006). Inactivation credit of UV radiation for viruses, bacteria and protozoan (oo)cysts in water: a review. Water Research, 40(1): 3–22

[21] Hua Z C, Li D, Wu Z H, Wang D, Cui Y L, Huang X F, Fang J Y, An T C. (2021). DBP formation and toxicity alteration during UV/chlorine treatment of wastewater and the effects of ammonia and bromide. Water Research, 188: 116549

[22] Huang W C, Du Y, Liu M, Hu H Y, Wu Q Y, Chen Y. (2019). Influence of UV irradiation on the toxicity of chlorinated water to mammalian cells: toxicity drivers, toxicity changes and toxicity surrogates. Water Research, 165: 115024

[23] Huang Y J, He Z X, Liao X B, Cheng Y S, Qi H. (2022). NDMA reduction mechanism of UDMH by O₃/PMS technology. Science of the Total Environment, 805: 150418

[24] Lazarova V, Savoye P, Janex M L, Blatchley E R III, Pommepuy M. (1999). Advanced wastewater disinfection technologies: state of the art and perspectives. Water Science and Technology, 40(4-5): 203–213

[25] Lei Y, Cheng S S, Luo N, Yang X, An T C. (2019). Rate constants and mechanisms of the reactions of Cl· and Cl₂·^– with trace organic contaminants. Environmental Science & Technology, 53(19): 11170–11182

[26] Li M K, Qiang Z M, Shi Y W. (2012). Research progress of effective radiation dose measurement methods for ultraviolet disinfection system. Journal of Environmental Sciences, 32(3): 513–520

[27] Liu D C, Rao L, Shi X Y, Du J Y, Chen C, Sun W J, Fu M L, Yuan B L. (2022). Comparison of the formation of N-nitrosodimethylamine (NDMA) from algae organic matter by chlor(am)ination and UV irradiation. Science of the Total Environment, 838: 156078

[28] Liu H B, Zhang X J, Fang Y Y, Fu C G, Chen Z B. (2021). Trade-off control of organic matter and disinfection by-products in the drinking water treatment chain: role of pre-ozonation. Science of the Total Environment, 770: 144767

[29] Liu J J, Liao X B, Zhou Z M, Li F, Yuan B L. (2015). Determination of seven N-nitrosamines in eutrophic drinking water after chlorination by high performance liquid chromatographytandem mass spectrometry. Chinese Journal of Analytical Chemistry, 43(4): 497–501

[30] Ma L F, Peng F Y, Dong Q Q, Li H P, Yang Z G. (2022). Identification of the key biochemical component contributing to disinfection byproducts in chlorinating algogenic organic matter. Chemosphere, 296: 133998

[31] Mortazavi M, Bains A, Afsah-Hejri L, Ehsani R, Liwang P J. (2022). SARS-CoV-2 pseudotyped virus persists on the surface of multiple produce but can be inactivated with gaseous ozone. Heliyon, 8(8): e10280

[32] Mundy B, Kuhnel B, Hunter G, Jarnis R, Funk D, Walker S, Burns N, Drago J, Nezgod W, Huang J. . (2018). A review of ozone systems costs for municipal applications. report by the municipal committee-IOA pan American group. Ozone Science and Engineering, 40(4): 266–274

[33] Murphy K R, Stedmon C A, Graeber D, Bro R. (2013). Fluorescence spectroscopy and multi-way techniques. PARAFAC. Analytical Methods, 5(23): 6557–6566

[34] Plewa M J, Wagner E D, Muellner M G. (2008). Comparative mammalian cell toxicity of N-DBPs and C-DBPs. ACS Symposium Series, 995: 36–50

[35] Ramseier M K, von Gunten U, Freihofer P, Hammes F. (2011). Kinetics of membrane damage to high (HNA) and low (LNA) nucleic acid bacterial clusters in drinking water by ozone, chlorine, chlorine dioxide, monochloramine, ferrate (VI), and permanganate. Water Research, 45(3): 1490–1500

[36] Roback S L, Ishida K P, Chuang Y, Zhang Z, Mitch W A, Plumlee M H. (2021). Pilot UV-AOP comparison of UV/hydrogen peroxide, UV/free chlorine, and UV/monochloramine for the removal of N-nitrosodimethylamine (NDMA) and NDMA Precursors. ACS ES&T Water, 1(2): 396–406

[37] Schroeder J P, Croot P L, Von Dewitz B, Waller U, Hanel R. (2011). Potential and limitations of ozone for the removal of ammonia, nitrite, and yellow substances in marine recirculating aquaculture systems. Aquacultural Engineering, 45(1): 35–41

[38] Sgroi M, Snyder S A, Roccaro P. (2021). Comparison of AOPs at pilot scale: energy costs for micro-pollutants oxidation, disinfection by-products formation and pathogens inactivation. Chemosphere, 273: 128527

[39] Shang C, Blatchley E R III. (2001). Chlorination of pure bacterial cultures in aqueous solution. Water Research, 35(1): 244–254

[40] Spiliotopoulou A, Rojas-Tirado P, Chhetri R K, Kaarsholm K M S, Martin R, Pedersen P B, Pedersen L, Andersen H R. (2018). Ozonation control and effects of ozone on water quality in recirculating aquaculture systems. Water Research, 133: 289–298

[41] Tian F X, Ye W K, Xu B, Hu X J, Ma S X, Lai F, Gao Y Q, Xing H B, Xia W H, Wang B. (2020). Comparison of UV-induced AOPs (UV/Cl, UV/NHCl, UV/ClO and UV/HO) in the degradation of iopamidol: kinetics, energy requirements and DBPs-related toxicity in sequential disinfection processes. Chemical Engineering Journal, 398: 125570

[42] Wagner E D, Plewa M J. (2017). CHO cell cytotoxicity and genotoxicity analyses of disinfection by-products: an updated review. Journal of Environmental Sciences-China, 58: 64–76

[43] WangD, Bolton J R, AndrewsS A, HofmannR (2015). Formation of disinfection by-products in the ultraviolet/chlorine advanced oxidation process. Science of the Total Environment, 518–519: 49–57

[44] Wang J, Liu X, Ng T W, Xiao J, Chow A T, Wong P K. (2013). Disinfection byproduct formation from chlorination of pure bacterial cells and pipeline biofilms. Water Research, 47(8): 2701–2709

[45] Wang J W, Shen J, Ye D, Yan X, Zhang Y J, Yang W J, Li X W, Wang J Q, Zhang L B, Pan L J. (2020). Disinfection technology of hospital wastes and wastewater: suggestions for disinfection strategy during coronavirus Disease 2019 (COVID-19) pandemic in China. Environmental Pollution, 262: 114665

[46] Wang L, Hu J Y. (2018). Formation of disinfection by-products in remineralized desalinated seawater with bacterial materials as precursor. Desalination, 441: 1–8

[47] Wang W L, Lee M Y, Du Y, Zhou T H, Yang Z W, Wu Q Y, Hu H Y. (2021). Understanding the influence of pre-ozonation on the formation of disinfection byproducts and cytotoxicity during post-chlorination of natural organic matter: UV absorbance and electron-donating-moiety of molecular weight fractions. Environment International, 157: 106793

[48] Wang W L, Wu Q Y, Huang N, Wang T, Hu H Y. (2016). Synergistic effect between UV and chlorine (UV/chlorine) on the degradation of carbamazepine: influence factors and radical species. Water Research, 98: 190–198

[49] Wang Z K, Kim J S, Seo Y W. (2012). Influence of bacterial extracellular polymeric substances on the formation of carbonaceous and nitrogenous disinfection byproducts. Environmental Science & Technology, 46(20): 11361–11369

[50] Wu Y W, Bu L J, Zhu S M, Chen F, Li T B, Zhou S Q, Shi Z. (2022). Molecular transformation of algal organic matter during sequential ozonation-chlorination: role of pre-ozonation and properties of chlorinated disinfection byproducts. Water Research, 223: 119008

[51] Wu Z H, Fang J Y, Xiang Y Y, Shang C, Li X C, Meng F G, Yang X. (2016). Roles of reactive chlorine species in trimethoprim degradation in the UV/chlorine process: kinetics and transformation pathways. Water Research, 104: 272–282

[52] Xiao R Y, Liu K, Bai L, Minakata D, Seo Y, Kaya Göktaş R, Dionysiou D D, Tang C J, Wei Z S, Spinney R. (2019). Inactivation of pathogenic microorganisms by sulfate radical: present and future. Chemical Engineering Journal, 371: 222–232

[53] Xiao Y J, Fan R L, Zhang L F, Yue J F, Webster R D, Lim T. (2014). Photodegradation of iodinated trihalomethanes in aqueous solution by UV₂₅₄ irradiation. Water Research, 49: 275–285

[54] Xie Y F. (2001). Analyzing haloacetic acids using gas chromatography/mass spectrometry. Water Research, 35(6): 1599–1602

[55] Yang X, Shang C. (2004). Chlorination byproduct formation in the presence of humic acid, model nitrogenous organic compounds, ammonia, and bromide. Environmental Science & Technology, 38(19): 4995–5001

[56] Zeber J E, Pfeiffer C, Baddley J W, Cadena-Zuluaga J, Stock E M, Copeland L A, Hendricks J, Mohammadi J, Restrepo M I, Jinadatha C. (2018). Effect of pulsed xenon ultraviolet room disinfection devices on microbial counts for methicillin-resistant Staphylococcus aureus and aerobic bacterial colonies. American Journal of Infection Control, 46(6): 668–673

[57] Zhang W J, Dong T Y, Ai J, Fu Q L, Zhang N, He H, Wang Q L, Wang D S. (2022). Mechanistic insights into the generation and control of Cl-DBPs during wastewater sludge chlorination disinfection process. Environment International, 167: 107389

[58] Zhang X N, Sun Y L, Ma F, Li A, Zhao H P, Wang A J, Yang J X. (2019). In-situ utilization of soluble microbial product (SMP) cooperated with enhancing SMP-dependent denitrification in aerobic-anoxic sequencing batch reactor. Science of the Total Environment, 693: 133558

[59] Zhou X, Ren X Y, Chen Y, Feng H P, Yu J F, Peng K, Zhang Y Y, Chen W H, Tang J, Wang J J. . (2023). Bacteria inactivation by sulfate radical: progress and non-negligible disinfection by-products. Frontiers of Environmental Science & Engineering, 17(3): 29

Acknowledgements

This work was financially supported by the Youth Science and Technology Innovation Program of Xiamen Ocean and Fisheries Development Special Funds (China) (No. 23YYST062QCB29). We would like to thank Instrumental Analysis Center of Huaqiao University (China) for intermediates detection using UPLC-QTOF/MS (Agilent 1290-6545, USA).

Conflict of Interests

The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest.

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11783-024-1875-5 and is accessible for authorized users.

RIGHTS & PERMISSIONS

2024 Higher Education Press 2024