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
1. Institute of Municipal and Environmental Engineering, College of Civil Engineering, Huaqiao University, Xiamen 361021, China 2. Xiamen Institute of Environmental Science, Xiamen 361021, China 3. College of Biomedical Sciences, Huaqiao University, Xiamen 361021, China
● 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.
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.
A A Abokifa, Y J Yang, C S Lo, P Biswas. (2016). Investigating the role of biofilms in trihalomethane formation in water distribution systems with a multicomponent model. Water Research, 104: 208–219 https://doi.org/10.1016/j.watres.2016.08.006
2
AWWA APHA, , 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
M T Aziz, C O Granger, D C Westerman, S P Putnam, J L Ferry, S D Richardson. (2022). Microseira wollei and Phormidium algae more than doubles DBP concentrations and calculated toxicity in drinking water. Water Research, 216: 118316 https://doi.org/10.1016/j.watres.2022.118316
4
E Bei, X Li, F H Wu, S X Li, X S He, Y F Wang, Y Qiu, Y Wang, C K Wang, J Wang. et al.. (2020). Formation of N-nitrosodimethylamine precursors through the microbiological metabolism of nitrogenous substrates in water. Water Research, 183: 116055 https://doi.org/10.1016/j.watres.2020.116055
5
T Beitz, W Bechmann, R Mitzner. (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
V J Black, C A Stewart, J A Roberts, C R Black. (2010). Direct effects of ozone on reproductive development in Plantago major L. populations differing in sensitivity. Environmental and Experimental Botany, 69(2): 121–128 https://doi.org/10.1016/j.envexpbot.2010.04.006
7
G Q Cai, T Z Liu, J S Zhang, H R Song, Q J Jiang, C Zhou. (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 https://doi.org/10.1016/j.watres.2022.118540
8
CDPH (2013). NDMA and Other Nitrosamines Drinking Water Issues. Sacramento, CA: California Department of Public Health
9
W Chen, P Westerhoff, J A Leenheer, K Booksh. (2003). Fluorescence excitation−emission matrix regional integration to quantify spectra for dissolved organic matter. Environmental Science & Technology, 37(24): 5701–5710 https://doi.org/10.1021/es034354c
10
X W Chen, Z Chen, H Liu, N Huang, Y Mao, K F Cao, Q Shi, Y Lu, H Y Hu. (2022). Synergistic effects of UV and chlorine in bacterial inactivation for sustainable water reclamation and reuse. Science of the Total Environment, 845: 157320 https://doi.org/10.1016/j.scitotenv.2022.157320
11
Y Q Chen, F Bai, Z Y Li, P C Xie, Z P Wang, X N Feng, Z Z Liu, L Z Huang. (2020). UV-assisted chlorination of algae-laden water: Cell lysis and disinfection byproducts formation. Chemical Engineering Journal, 383: 123165 https://doi.org/10.1016/j.cej.2019.123165
12
X L Ding, J Y Zhu, J Zhang, T Y Dong, Y K Xia, J D Jiao, X R Wang, W J Zhou. (2020). Developmental toxicity of disinfection by-product monohaloacetamides in embryo-larval stage of zebrafish. Ecotoxicology and Environmental Safety, 189: 110037 https://doi.org/10.1016/j.ecoenv.2019.110037
13
F L Dong, Q F Lin, C Li, L P Wang, A García. (2021). UV/chlorination process of algal-laden water: algal inactivation and disinfection byproducts attenuation. Separation and Purification Technology, 257: 117896 https://doi.org/10.1016/j.seppur.2020.117896
14
X C Duan, X B Liao, J Chen, S G Xie, H Qi, F Li, B L Yuan. (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 https://doi.org/10.1016/j.scitotenv.2020.140833
15
J Y Fang, Y Fu, C Shang. (2014). The roles of reactive species in micropollutant degradation in the UV/free chlorine system. Environmental Science & Technology, 48(3): 1859–1868 https://doi.org/10.1021/es4036094
16
Z C Gao, Y L Lin, B Xu, Y Xia, C Y Hu, T Y Zhang, H Qian, T C Cao, N Y Gao. (2020). Effect of bromide and iodide on halogenated by-product formation from different organic precursors during UV/chlorine processes. Water Research, 182: 116035 https://doi.org/10.1016/j.watres.2020.116035
17
A M Gorito, A R L Ribeiro, P Rodrigues, M F R Pereira, L Guimarães, C M R Almeida, A M T Silva. (2022). Antibiotics removal from aquaculture effluents by ozonation: chemical and toxicity descriptors. Water Research, 218: 118497 https://doi.org/10.1016/j.watres.2022.118497
18
K H Guo, Z H Wu, C Shang, B Yao, S D Hou, X Yang, W H Song, J Y Fang. (2017). Radical chemistry and structural relationships of PPCP degradation by UV/chlorine treatment in simulated drinking water. Environmental Science & Technology, 51(18): 10431–10439 https://doi.org/10.1021/acs.est.7b02059
19
M T Guo, J J Huang, H Y Hu, W J Liu. (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
W A M Hijnen, E F Beerendonk, G J Medema. (2006). Inactivation credit of UV radiation for viruses, bacteria and protozoan (oo)cysts in water: a review. Water Research, 40(1): 3–22 https://doi.org/10.1016/j.watres.2005.10.030
21
Z C Hua, D Li, Z H Wu, D Wang, Y L Cui, X F Huang, J Y Fang, T C An. (2021). DBP formation and toxicity alteration during UV/chlorine treatment of wastewater and the effects of ammonia and bromide. Water Research, 188: 116549 https://doi.org/10.1016/j.watres.2020.116549
22
W C Huang, Y Du, M Liu, H Y Hu, Q Y Wu, Y Chen. (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 https://doi.org/10.1016/j.watres.2019.115024
23
Y J Huang, Z X He, X B Liao, Y S Cheng, H Qi. (2022). NDMA reduction mechanism of UDMH by O3/PMS technology. Science of the Total Environment, 805: 150418 https://doi.org/10.1016/j.scitotenv.2021.150418
24
V Lazarova, P Savoye, M L Janex, E R III Blatchley, M Pommepuy. (1999). Advanced wastewater disinfection technologies: state of the art and perspectives. Water Science and Technology, 40(4-5): 203–213 https://doi.org/10.2166/wst.1999.0593
25
Y Lei, S S Cheng, N Luo, X Yang, T C An. (2019). Rate constants and mechanisms of the reactions of Cl· and Cl2·– with trace organic contaminants. Environmental Science & Technology, 53(19): 11170–11182 https://doi.org/10.1021/acs.est.9b02462
26
M K Li, Z M Qiang, Y W Shi. (2012). Research progress of effective radiation dose measurement methods for ultraviolet disinfection system. Journal of Environmental Sciences, 32(3): 513–520
27
D C Liu, L Rao, X Y Shi, J Y Du, C Chen, W J Sun, M L Fu, B L Yuan. (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 https://doi.org/10.1016/j.scitotenv.2022.156078
28
H B Liu, X J Zhang, Y Y Fang, C G Fu, Z B Chen. (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 https://doi.org/10.1016/j.scitotenv.2020.144767
29
J J Liu, X B Liao, Z M Zhou, F Li, B L Yuan. (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
L F Ma, F Y Peng, Q Q Dong, H P Li, Z G Yang. (2022). Identification of the key biochemical component contributing to disinfection byproducts in chlorinating algogenic organic matter. Chemosphere, 296: 133998 https://doi.org/10.1016/j.chemosphere.2022.133998
31
M Mortazavi, A Bains, L Afsah-Hejri, R Ehsani, P J Liwang. (2022). SARS-CoV-2 pseudotyped virus persists on the surface of multiple produce but can be inactivated with gaseous ozone. Heliyon, 8(8): e10280 https://doi.org/10.1016/j.heliyon.2022.e10280
32
B Mundy, B Kuhnel, G Hunter, R Jarnis, D Funk, S Walker, N Burns, J Drago, W Nezgod, J Huang. et al.. (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 https://doi.org/10.1080/01919512.2018.1467187
33
K R Murphy, C A Stedmon, D Graeber, R Bro. (2013). Fluorescence spectroscopy and multi-way techniques. PARAFAC. Analytical Methods, 5(23): 6557–6566 https://doi.org/10.1039/c3ay41160e
34
M J Plewa, E D Wagner, M G Muellner. (2008). Comparative mammalian cell toxicity of N-DBPs and C-DBPs. ACS Symposium Series, 995: 36–50
35
M K Ramseier, U von Gunten, P Freihofer, F Hammes. (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 https://doi.org/10.1016/j.watres.2010.11.016
36
S L Roback, K P Ishida, Y Chuang, Z Zhang, W A Mitch, M H Plumlee. (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 https://doi.org/10.1021/acsestwater.0c00155
37
J P Schroeder, P L Croot, B Von Dewitz, U Waller, R Hanel. (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 https://doi.org/10.1016/j.aquaeng.2011.06.001
38
M Sgroi, S A Snyder, P Roccaro. (2021). Comparison of AOPs at pilot scale: energy costs for micro-pollutants oxidation, disinfection by-products formation and pathogens inactivation. Chemosphere, 273: 128527 https://doi.org/10.1016/j.chemosphere.2020.128527
A Spiliotopoulou, P Rojas-Tirado, R K Chhetri, K M S Kaarsholm, R Martin, P B Pedersen, L Pedersen, H R Andersen. (2018). Ozonation control and effects of ozone on water quality in recirculating aquaculture systems. Water Research, 133: 289–298 https://doi.org/10.1016/j.watres.2018.01.032
41
F X Tian, W K Ye, B Xu, X J Hu, S X Ma, F Lai, Y Q Gao, H B Xing, W H Xia, B Wang. (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 https://doi.org/10.1016/j.cej.2020.125570
42
E D Wagner, M J Plewa. (2017). CHO cell cytotoxicity and genotoxicity analyses of disinfection by-products: an updated review. Journal of Environmental Sciences-China, 58: 64–76 https://doi.org/10.1016/j.jes.2017.04.021
43
D Wang, J R Bolton, S A Andrews, R Hofmann (2015). Formation of disinfection by-products in the ultraviolet/chlorine advanced oxidation process. Science of the Total Environment, 518–519: 49–57
44
J Wang, X Liu, T W Ng, J Xiao, A T Chow, P K Wong. (2013). Disinfection byproduct formation from chlorination of pure bacterial cells and pipeline biofilms. Water Research, 47(8): 2701–2709 https://doi.org/10.1016/j.watres.2013.02.038
45
J W Wang, J Shen, D Ye, X Yan, Y J Zhang, W J Yang, X W Li, J Q Wang, L B Zhang, L J Pan. (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 https://doi.org/10.1016/j.envpol.2020.114665
46
L Wang, J Y Hu. (2018). Formation of disinfection by-products in remineralized desalinated seawater with bacterial materials as precursor. Desalination, 441: 1–8 https://doi.org/10.1016/j.desal.2018.04.022
47
W L Wang, M Y Lee, Y Du, T H Zhou, Z W Yang, Q Y Wu, H Y Hu. (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 https://doi.org/10.1016/j.envint.2021.106793
48
W L Wang, Q Y Wu, N Huang, T Wang, H Y Hu. (2016). Synergistic effect between UV and chlorine (UV/chlorine) on the degradation of carbamazepine: influence factors and radical species. Water Research, 98: 190–198 https://doi.org/10.1016/j.watres.2016.04.015
49
Z K Wang, J S Kim, Y W Seo. (2012). Influence of bacterial extracellular polymeric substances on the formation of carbonaceous and nitrogenous disinfection byproducts. Environmental Science & Technology, 46(20): 11361–11369 https://doi.org/10.1021/es301905n
50
Y W Wu, L J Bu, S M Zhu, F Chen, T B Li, S Q Zhou, Z Shi. (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 https://doi.org/10.1016/j.watres.2022.119008
51
Z H Wu, J Y Fang, Y Y Xiang, C Shang, X C Li, F G Meng, X Yang. (2016). Roles of reactive chlorine species in trimethoprim degradation in the UV/chlorine process: kinetics and transformation pathways. Water Research, 104: 272–282 https://doi.org/10.1016/j.watres.2016.08.011
52
R Y Xiao, K Liu, L Bai, D Minakata, Y Seo, Göktaş R Kaya, D D Dionysiou, C J Tang, Z S Wei, R Spinney. (2019). Inactivation of pathogenic microorganisms by sulfate radical: present and future. Chemical Engineering Journal, 371: 222–232 https://doi.org/10.1016/j.cej.2019.03.296
53
Y J Xiao, R L Fan, L F Zhang, J F Yue, R D Webster, T Lim. (2014). Photodegradation of iodinated trihalomethanes in aqueous solution by UV254 irradiation. Water Research, 49: 275–285 https://doi.org/10.1016/j.watres.2013.11.039
X Yang, C Shang. (2004). Chlorination byproduct formation in the presence of humic acid, model nitrogenous organic compounds, ammonia, and bromide. Environmental Science & Technology, 38(19): 4995–5001 https://doi.org/10.1021/es049580g
56
J E Zeber, C Pfeiffer, J W Baddley, J Cadena-Zuluaga, E M Stock, L A Copeland, J Hendricks, J Mohammadi, M I Restrepo, C Jinadatha. (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 https://doi.org/10.1016/j.ajic.2018.02.001
57
W J Zhang, T Y Dong, J Ai, Q L Fu, N Zhang, H He, Q L Wang, D S Wang. (2022). Mechanistic insights into the generation and control of Cl-DBPs during wastewater sludge chlorination disinfection process. Environment International, 167: 107389 https://doi.org/10.1016/j.envint.2022.107389
58
X N Zhang, Y L Sun, F Ma, A Li, H P Zhao, A J Wang, J X Yang. (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 https://doi.org/10.1016/j.scitotenv.2019.07.364
59
X Zhou, X Y Ren, Y Chen, H P Feng, J F Yu, K Peng, Y Y Zhang, W H Chen, J Tang, J J Wang. et al.. (2023). Bacteria inactivation by sulfate radical: progress and non-negligible disinfection by-products. Frontiers of Environmental Science & Engineering, 17(3): 29
