Applied Chemical Engineering

Removal of trace organic pollutants and generation of halogenated disinfection by-products in membrane UV/chlorine combined process

Yafei Yu

School of Environmental Science and Engineering, Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Sun Yat-sen University

Yu Lei

School of Environmental Science and Engineering, Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Sun Yat-sen University

Mengge Fan

School of Environmental Science and Engineering, Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Sun Yat-sen University

Xin Lei

School of Environmental Science and Engineering, Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Sun Yat-sen University

Shanshan Zhao

School of Environmental Science and Engineering, Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Sun Yat-sen University

Xin Yang

School of Environmental Science and Engineering, Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Sun Yat-sen University

DOI: https://doi.org/10.24294/ace.v5i1.1634

Keywords: UV/Chlorine, Trace Organic Pollutants, Halogenated Disinfection By-Products, Membrane Pretreatment, Dissolved Organic Matter

---

Abstract

In this study, the degradation kinetics and degradation mechanism of 23 trace organic pollutants (TrOCs) in the secondary effluent of sewage by the combined membrane-UV/chlorine process were investigated, and the halogenated disinfection by-products (X-DBPs) in the combined process were investigated and its generation potential (X-DBPsFP), and the cytotoxicity and genotoxicity of the treated water samples were also evaluated. The results showed that membrane pretreatment could effectively promote the degradation of TrOCs in UV/chlorine system, and nanofiltration (NF) was more effective than ultrafiltration (UF). Compared with UF, NF intercepts more dissolved organic matter (DOM), thus weakening the light shielding effect, chlorine consumption and radical quenching to a greater extent. It is found that the degradation mechanism of TrOCs can be divided into the following four categories: Ho˙ dominated, RHS dominated, chlorine and RHS jointly dominated and chlorine dominated. Membrane pretreatment can well reduce the formation of X-DBPs, among which UF and NF reduce the formation of haloacetamide (HAMs) and trihalomethanes (THMs) most significantly, while NF reduces the formation of X-DBPs and X-DBPsFP and the toxicity of water samples much stronger than UF. In addition, NF UV/chlorine can significantly remove the precursors of X-DBPs, so as to effectively control the enhancement of cytotoxicity and genotoxicity of water samples in the post chlorination process. The research results promote the development of advanced sewage treatment technology and provide theoretical guidance for related research.

---

References

[1] Esplugas S, Bila DM, Krause LGT, et al. Ozonation and advanced oxidation technologies to remove endocrine disrupting chemicals (EDCs) and pharmaceuticals and personal care products (PPCPs) in water effluents. Journal of Hazardous Materials 2007; 149(3): 631–642.

[2] Pan X, Qiang Z, Wang W. Distribution and ecological risk of sedimentary PPCPs in the eastern drinking water source area of Chaohu Lake. Environmental Chemistry 2016; 35(11): 2234–2244.

[3] Roberts J, Kumar A, Du J, et al. Pharmaceuticals and personal care products (PPCPs) in Australia’s largest inland sewage treatment plant, and its contribution to a major Australian river during high and low flow. Science of the Total Environment 2016; 541: 1625–1637.

[4] Peng X, Ou W, Wang C, et al. Occurrence and ecological potential of pharmaceuticals and personal care products in groundwater and reservoirs in the vicinity of municipal landfills in China. Science of the Total Environment 2014; 490: 889–898.

[5] Wee SY, Aris AZ, Yusoff FM, et al. Occurrence and risk assessment of multiclass endocrine disrupting compounds in an urban tropical river and a proposed risk management and monitoring framework. Science of the Total Environment 2019; 671: 431–442.

[6] Brausch JM, Rand GM. A review of personal care products in the aquatic environment: Environmental concentrations and toxicity. Chemosphere 2011; 82(11): 1518–1532.

[7] Lupo A, Coyne S, Berendonk TU. Origin and evolution of antibiotic resistance: The common mechanisms of emergence and spread in water bodies. Frontiers in Microbiology 2012; 3: 18.

[8] Feng T, Huang Y, Pan Y, et al. Degradation of acetaminophen and toxicity evaluation of the degradation products under three oxidation processes. Environmental Chemistry 2019; 38(1): 23–33.

[9] Ouyang Z, Huang Z, Tang X, et al. A dually charged nanofiltration membrane by pH-responsive polydopamine for pharmaceuticals and personal care products removal. Separation and Purification Technology 2019; 211: 90–97.

[10] Chuang YH, Chen S, Chinn CJ, et al. Comparing the UV/monochloramine and UV/free chlorine advanced oxidation processes (AOPs) to the UV/hydrogen peroxide AOP under scenarios relevant to potable reuse. Environmental Science & Technology 2017; 51(23): 13859–13868.

[11] Guo K, Wu Z, Yan S, et al. Comparison of the UV/chlorine and UV/H2O2 processes in the degradation of PPCPs in simulated drinking water and wastewater: Kinetics, radical mechanism and energy requirements. Water Research 2018; 147: 184–194.

[12] Xiang Y, Fang J, Shang C. Kinetics and pathways of ibuprofen degradation by the UV/chlorine advanced oxidation process. Water Research 2016; 90: 301–308.

[13] Guo K, Wu Z, Shang C, et al. Radical chemistry and structural relationships of PPCP degradation by UV/chlorine treatment in simulated drinking water. Environmental Science & Technology 2017; 51(18): 10431–10439.

[14] Wang W, Zhang X, Wu Q, et al. Degradation of natural organic matter by UV/chlorine oxidation: Molecular decomposition, formation of oxidation byproducts and cytotoxicity. Water Research 2017; 124: 251–258.

[15] Ahmed AE, Campbell GA, Jacob S. Neurological impairment in fetal mouse brain by drinking water disinfectant byproducts. NeuroToxicology 2005; 26(4): 633–640.

[16] Bove F, Shim Y, Zeitz P. Drinking water contaminants and adverse pregnancy outcomes: A review. Environmental Health Perspectives 2002; 110(Suppl.1): 61–74.

[17] Bull RJ, Meier JR, Robinson M, et al. Evaluation of mutagenic and carcinogenic properties of brominated and chlorinated acetonitriles: By-products of chlorination. Toxicological Sciences 1985; 5(6): 1065–1074.

[18] Rubia Á de la, Rodríguez M, León VM, et al. Removal of natural organic matter and THM formation potential by ultra- and nanofiltration of surface water. Water Research 2008; 42(3): 714–722.

[19] Rice EW, Baird RB, Eaton AD, et al. Standard methods for the examination of water and wastewater. 22nd ed. Washington: American Public Health Association (APHA), American Water Works Association (AWWA), Water Environment Federation (WEF); 2012.

[20] Lei Y, Cheng S, Luo N, et al. Rate constants and mechanisms of the reactions of Cl˙ and Cl2˙− with trace organic contaminants. Environmental Science & Technology 2019; 53(19): 11170–11182.

[21] Munch DJ, Hautman DP. Method 551.1: Determination of chlorination disinfection byproducts, chlorinated solvents, and halogenated pesticides/herbicides in drinking water by liquid-liquid extraction and gas chromatography with electron-capture detection. U.S. Environment Protection Agency; 1995.

[22] Chuang YH, Szczuka A, Shabani F, et al. Pilot-scale comparison of microfiltration/reverse osmosis and ozone/biological activated carbon with UV/hydrogen peroxide or UV/free chlorine AOP treatment for controlling disinfection byproducts during wastewater reuse. Water Research 2019; 152: 215–225.

[23] Wagner ED, Plewa MJ. CHO cell cytotoxicity and genotoxicity analyses of disinfection by-products: An updated review. Journal of Environmental Sciences 2017; 58: 64–76.

[24] Westerhoff P, Chao P, Mash H. Reactivity of natural organic matter with aqueous chlorine and bromine. Water Research 2004; 38(6): 1502–1513.

[25] Lei Y, Lei X, Westerhoff P, et al. Reactivity of chlorine radicals (Cl˙ and Cl2˙−) with dissolved organic matter and the formation of chlorinated byproducts. Environmental Science & Technology 2021; 55(1): 689–699.

[26] Guo K, Zheng S, Zhang X, et al. Roles of bromine radicals and hydroxyl radicals in the degradation of micropollutants by the UV/bromine process. Environmental Science & Technology 2020; 54(10): 6415–6426.

[27] Laurentiis ED, Minella M, Maurino V, et al. Assessing the occurrence of the dibromide radical (Br2˙− in natural waters: Measures of triplet-sensitised formation, reactivity, and modelling. Science of the Total Environment 2012; 439: 299–306.

[28] Canonica S, Kohn T, Mac M, et al. Photosensitizer method to determine rate constants for the reaction of carbonate radical with organic compounds. Environmental Science & Technology 2005; 39(23): 9182–9188.

[29] Wols BA, Hofman-Caris CHM. Review of photochemical reaction constants of organic micropollutants required for UV advanced oxidation processes in water. Water Research 2012; 46(9): 2815–2827.

[30] Zhou Y, Chen C, Guo K, et al. Kinetics and pathways of the degradation of PPCPs by carbonate radicals in advanced oxidation processes. Water Research 2020; 185: 116231.

[31] Lei Y, Lei X, Yu Y, et al. Rate constants and mechanisms for reactions of bromine radicals with trace organic contaminants. Environmental Science & Technology 2021; 55(15): 10502–10513.

[32] Márquez G, Rodríguez EM, Beltrán FJ, et al. Determination of rate constants for ozonation of ofloxacin in aqueous solution. Ozone: Science & Engineering 2013; 35(3): 186–195.

[33] Wang HJ, Mustafa M, Yu G, et al. Oxidation of emerging biocides and antibiotics in wastewater by ozonation and the electro-peroxone process. Chemosphere 2019; 235: 575–585.

[34] Razavi B, Song WH, Cooper WJ, et al. Free-radical-induced oxidative and reductive degradation of fibrate pharmaceuticals: Kinetic studies and degradation mechanisms. The Journal of Physical Chemistry A 2009; 113(7): 1287–1294.

[35] Huang Y, Kong MH, Westerman D, et al. Effects of HCO3− on degradation of toxic contaminants of emerging concern by UV/NO3−. Environmental Science & Technology 2018; 52(21): 12697–12707.

[36] Dodd MC, Buffle MO, Von Gunten U. Oxidation of antibacterial molecules by aqueous ozone: Moiety-specific reaction kinetics and application to ozone-based wastewater treatment. Environmental Science & Technology 2006; 40(6): 1969–1977.

[37] Lian L, Yao B, Hou S, et al. Kinetic study of hydroxyl and sulfate radical-mediated oxidation of pharmaceuticals in wastewater effluents. Environmental Science & Technology 2017; 51(5): 2954–2962.

[38] Kong X, Wang L, Wu Z, et al. Solar irradiation combined with chlorine can detoxify herbicides. Water Research 2020; 177: 115784.

[39] Song WH, Cooper WJ, Mezyk SP, et al. Free radical destruction of β-blockers in aqueous solution. Environmental Science & Technology 2008; 42(4): 1256–1261.

[40] Wols BA, Harmsen DJH, Wanders-Dijk J, et al. Degradation of pharmaceuticals in UV(LP)/H2O2 reactors simulated by means of kinetic modeling and computational fluid dynamics (CFD). Water Research 2015; 75: 11–24.

[41] Sunil Paul MM, Aravind UK, Pramod G, et al. Hydroxyl radical induced oxidation of theophylline in water: A kinetic and mechanistic study. Organic & Biomolecular Chemistry 2014; 12(30): 5611–5620.

[42] Deborde M, Von Gunten U. Reactions of chlorine with inorganic and organic compounds during water treatment—Kinetics and mechanisms: A critical review. Water Research 2008; 42(1/2): 13–51.

[43] Bond T, Huang J, Templeton MR, et al. Occurrence and control of nitrogenous disinfection by-products in drinking water: A review. Water Research 2011; 45(15): 4341–4354.

[44] Xiang H, Shao Y, Gao N, et al. Removal of β-cyclocitral by UV/persulfate and UV/chlorine process: Degradation kinetics and DBPs formation. Chemical Engineering Journal 2020; 382: 122659.

[45] Xie P, Ma J, Liu W, et al. Impact of UV/persulfate pretreatment on the formation of disinfection byproducts during subsequent chlorination of natural organic matter. Chemical Engineering Journal 2015; 269: 203–211.