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Frontiers of Environmental Science & Engineering

ISSN 2095-2201

ISSN 2095-221X(Online)

CN 10-1013/X

Postal Subscription Code 80-973

2018 Impact Factor: 3.883

Front. Environ. Sci. Eng.    2021, Vol. 15 Issue (5) : 93    https://doi.org/10.1007/s11783-020-1338-6
RESEARCH ARTICLE
Characteristics and removal mechanism of the precursors of N-chloro-2,2-dichloroacetamide in a drinking water treatment process at Taihu Lake
Mengqing Ge1,2, Tao Lin1,2(), Kemei Zhou3, Hong Chen4, Hang Xu1,2, Hui Tao1,2, Wei Chen1,2
1. Ministry of Education Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes, Hohai University, Nanjing 210098, China
2. College of Environment, Hohai University, Nanjing 210098, China
3. Nanjing Water Group Company Limited, Nanjing 210002, China
4. Soil and Environmental Analysis and Testing Center, Nanjing Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, China
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Abstract

• N-Cl-DCAM, an emerging N-DBP in drinking water was investigated.

• A new BAC has a better removal efficiency for N-Cl-DCAM precursors than an old BAC.

• N-Cl-DCAM precursors are more of low molecular weight and non-polar.

• Adsorption of GAC plays a major role in removal of N-Cl-DCAM precursors by an O3-BAC.

N-chloro-2,2-dichloroacetamide (N-Cl-DCAM) is an emerging nitrogenous disinfection by-product (N-DBP) which can occur in drinking water. In this study, an analytical method based on liquid chromatography with tandem mass spectrometry (LC-MS/MS) was developed to validate the concentration of N-Cl-DCAM, which was found to be 1.5 mg/L in the effluent of a waterworks receiving raw water from Taihu Lake, China. The changes of N-Cl-DCAM formation potential (N-Cl-DCAMFP) in the drinking water treatment process and the removal efficiency of its precursors in each unit were evaluated. Non-polar organics accounted for the majority of N-Cl-DCAM precursors, accounting for 70% of the N-Cl-DCAM FP. The effect of conventional water treatment processes on the removal of N-Cl-DCAM precursors was found to be unsatisfactory due to their poor performance in the removal of low molecular weight (MW) or non-polar organics. In the ozonation integrated with biological activated carbon (O3-BAC) process, the ozonation had little influence on the decrease of N-Cl-DCAM FP. The removal efficiency of precursors by a new BAC filter, in which the granular activated carbon (GAC) had only been used for four months was higher than that achieved by an old BAC filter in which the GAC had been used for two years. The different removal efficiencies of precursors were mainly due to the different adsorption capacities of GAC for individual precursors. Low MW or non-polar organics were predominantly removed by GAC, rather than biodegradation by microorganisms attached to GAC particles.

Keywords N-chloro-2,2-dichloroacetamide      Liquid chromatography with tandem mass spectrometry      Precursors      Removal efficiency      Ozonation integrated with biological activated carbon     
Corresponding Author(s): Tao Lin   
Issue Date: 17 December 2020
 Cite this article:   
Mengqing Ge,Tao Lin,Kemei Zhou, et al. Characteristics and removal mechanism of the precursors of N-chloro-2,2-dichloroacetamide in a drinking water treatment process at Taihu Lake[J]. Front. Environ. Sci. Eng., 2021, 15(5): 93.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-020-1338-6
https://academic.hep.com.cn/fese/EN/Y2021/V15/I5/93
Fig.1  N-Chloro-2,2-dichloroacetamide (N-Cl-DCAM) (MW= 162.5 g/mol).
Parameters Value
Turbidity (NTU) 18±1.44
UV254 (cm1) 0.064±0.007
CODMn (mg/L) 4.07±0.32
NH3-N (mg/L) 0.142±0.011
DOC (mg/L) 5.30±0.39
DON (mg/L) 0.278±0.028
Br? (µg/L) 113±16
Tab.1  The water quality characteristics of Taihu Lake
Fig.2  A process diagram of the waterworks.
Parameters Value
New GAC Old GAC
Usage time of GAC 4 months 2 years
Particle size (%)
>1.70 mm
1.70–0.425 mm
<0.425 mm
0.2
99.3
0.1
99.5
0.5 0.4
Pore volume (mL/g) 0.65 0.55
Specific surface area (m2/g) 810 760
Biomass (nmol/g) 92 97
Biological activity (mg·O2/(L·cm3)) 43.2 47.6
Iodine adsorption (mg/g) 914 856
Methylene blue adsorption (mg/g) 224 183
Tab.2  The characteristics of the new and old GAC used in the BAC filters
Fig.3  Standard calibration graph for N-Cl-DCAM.
Fig.4  Total ion flow chromatogram of a 5 mg/L N-Cl-DCAM standard solution.
Samples AB 5500LC-MS/MS (mg/L) SPE-UPLC/ESI/qTOF (mg/L)
Raw water 5.55±0.30 5.69±0.29
Pre-ozonation 5.26±0.22 5.12±0.18
Sedimentation 4.57±0.25 4.67±0.27
Post-ozonation 4.29±0.20 4.15±0.16
New BAC 1.67±0.11 1.53±0.13
Old BAC 3.01±0.15 3.14±0.12
Tab.3  A comparison of the N-Cl-DCAM FP obtained using the LC-MS/MS method and the UPLC/TOFMS method
Fig.5  Total ion flow chromatogram of raw water.
Fig.6  The N-Cl-DCAN FP in the effluent of different processes.
Fig.7  Relative abundances of bacterial genera on the new and old BAC.
Samples N-Cl-DCAM FP (mg/L)
Effluent of post-ozone contact tank 4.3±0.2
New carbon
Effluent of biological activated carbon filters 1.7±0.1
Effluent of inactivated carbon filters 1.9±0.1
Old carbon
Effluent of biological activated carbon filters 3.0±0.2
Effluent of inactivated carbon filters 3.3±0.2
Tab.4  Removal of N-Cl-DCAM FP by biological activated carbon and inactivated carbon
Samples N-Cl-DCAM FP
(mg/L)
MW<1 kDa
(mg/L)
MW= 1–3 kDa
(mg/L)
MW= 3–10 kDa
(mg/L)
MW>10 kDa
(mg/L)
Raw water 5.6±0.3 2.2±0.2 1.6±0.2 0.7±0.1 1.1±0.1
Pre-ozone 5.3±0.2 2.2±0.2 1.5±0.1 0.6±0.1 0.9±0.1
Sedimentation 4.6±0.3 1.8±0.1 1.3±0.1 0.6±0.1 0.8±0.1
Post-ozone 4.3±0.2 1.8±0.2 1.2±0.1 0.5±0.1 0.8±0.1
New BAC 1.7±0.1 0.7±0.1 0.4±0.1 0.2±0.1 0.4±0.1
Old BAC 3.0±0.2 1.3±0.1 0.8±0.1 0.4±0.1 0.5±0.1
Tab.5  The MW distribution of N-Cl-DCAM precursors in the different processes
Fig.8  The MW distribution of organic matter in the effluent of new and old BAC filters.
Samples MW<1 kDa
(mg/L)
MW= 1–3 kDa
(mg/L)
MW= 3–10 kDa
(mg/L)
MW>10 kDa
(mg/L)
New carbon
Effluent of biological activated carbon filters 0.7±0.1 0.4±0.1 0.2±0.1 0.4±0.1
Effluent of inactivated carbon filters 0.8±0.1 0.5±0.1 0.3±0.2 0.4±0.1
Old carbon
Effluent of biological activated carbon filters 1.3±0.1 0.8±0.1 0.4±0.1 0.5±0.2
Effluent of inactivated carbon filters 1.4±0.1 0.9±0.2 0.4±0.1 0.6±0.1
Tab.6  Removal of different MW N-Cl-DCAM precursors by biological activated carbon and inactivated carbon
Samples DOC (mg/L) N-Cl-DCAM FP (mg/L)
Raw water 4.9±0.3 5.6±0.3
Non-polar 2.9±0.2 3.9±0.3
Polar 1.9±0.2 1.7±0.1
Tab.7  Polar and non-polar properties of N-Cl-DCAM precursors
Samples N-Cl-DCAM FP (mg/L) Non-polar (mg/L) Polar (mg/L)
Raw water 5.6±0.3 3.4±0.3 1.7±0.1
Pre-ozone 5.3±0.2 3.7±0.3 1.6±0.1
Sedimentation 4.6±0.3 3.2±0.2 1.4±0.1
Post-ozone 4.3±0.2 2.6±0.2 1.7±0.2
New BAC 1.7±0.1 0.9±0.1 0.8±0.1
Old BAC 3.0±0.2 1.8±0.1 1.2±0.1
Tab.8  The polar and non-polar properties of N-Cl-DCAM precursors in the different processes
Fig.9  Polarity and non-polarity of organic matter in the effluent of new and old BAC filters.
Samples Non-polar
(mg/L)
Polar
(mg/L)
New BAC
Effluent of inactivated carbon filters 1.1±0.1 0.89±0.1
Effluent of biological activated carbon filters 0.9±0.1 0.8±0.1
Old BAC
Effluent of inactivated carbon filters 2.0±0.2 1.3±0.1
Effluent of biological activated carbon filters 1.8±0.1 1.2±0.1
Tab.9  Removal of polar and non-polar organics of N-Cl-DCAM precursors by biological activated carbon and inactivated carbon
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