Ye Du

Differences in dissolved organic matter between reclaimed water source and drinking water source

Dissolved organic matter (DOM) significantly affects the quality of reclaimed water and drinking water. Reclaimed water potable reuse is an effective way to augment drinking water source and de facto reuse exists worldwide. Hence, when reclaimed water source (namely secondary effluent) is blended with drinking water source, understanding the difference in DOM between drinking water source (dDOM) and reclaimed water source (rDOM) is essential. In this study, composition, transformation, and potential risk of dDOM from drinking water source and rDOM from secondary effluent were compared. Generally, the DOC concentration of rDOM and dissolved organic nitrogen (DON) content in reclaimed water source were higher but rDOM exhibited a lower aromaticity. Besides, rDOM comprises a higher proportion of hydrophilic fractions and more low-molecular weight compounds, which are difficult to be removed during coagulation. Although dDOM exhibited higher specific disinfection byproducts formation potential (SDBPFP), rDOM formed more total disinfection byproducts (DBPs) during chlorination including halomethanes (THMs) and haloacetic acids (HAAs) due to high DOC concentration. Likewise, in consideration of DOC basis, rDOM contained more absolute assimilable organic carbon (AOC) despite showing a lower specific AOC (normalized AOC per unit of DOC). Besides, rDOM exhibited higher biotoxicity including genotoxicity and endocrine disruption. Therefore, rDOM presents a greater potential risk than dDOM does. Reclaimed water source needs to be treated carefully when it is blended with drinking water source.

Transformation of anti-estrogenic-activity related dissolved organic matter in secondary effluents during ozonation

Anti-estrogenic activity of dissolved organic matter (DOM) in reclaimed water is gaining increasing attention. In this study, anti-estrogenic activity removal efficiency by ozonation in the tertiary treatment process of domestic wastewater was investigated. The anti-estrogenic activity in the secondary effluents used in this study ranged between 0.95 and 2.00 mg-TAM L(-1) and decreased significantly after ozonation. The removal efficiency of anti-estrogenic activity at a dose of 10 mg-O3 L(-1) was 65-87%. The removal of the anti-estrogenic activity was highly correlated with the removal of UV254, suggesting that UV254 can be used as a surrogate for anti-estrogenic activity during ozonation. The results of size exclusion chromatography of the wastewater samples during ozonation showed that the UV254 absorbance of the DOM fraction with large apparent molecular weight (MW) around 7.6 k Da dropped significantly, and the DOM fraction was suspected to be humic substances which have been previously identified as anti-estrogenic constituents in secondary effluents. The excitation emission matrix fluorescence spectra of the wastewater samples proved that humic substances existed in the DOM and indeed reacted with the ozone. With the help of two-dimensional correlation of Fourier transform infrared, it was confirmed that the aromatic structures in the DOM were largely destroyed by ozonation. Therefore, it was suggested that the destruction of the aromatic structures in the DOM was related to the removal of the anti-estrogenic activity.

Anti-estrogenic activity formation potential assessment and precursor analysis in reclaimed water during chlorination

Chlorination was reported to increase the anti-estrogenic activity in reclaimed water from domestic wastewater treatment plants, which may add to the risk of reclaimed water reuse. In order to assess the anti-estrogenic disinfection by-product (DBP) precursors, the anti-estrogenic activity formation potential (AEAFP) during chlorination was studied. Firstly, the conditions for the experimental measurement of AEAFP were determined. A 24-h chlorination experiment was applied for AEAFP measurement. After chlorination, dechlorination using reductive reagents led to significant loss of anti-estrogenic activity formation. In addition, as the presence of ammonia nitrogen and other major chlorine consumers would result in lower anti-estrogenic activity formation, a basic chlorine dose of 3× DOC (mg-Cl2 L(-1)) was adequate for completely transforming the anti-estrogenic DBP precursors while an extra chlorine dose of 8× ammonia-nitrogen + 5× nitrite-nitrogen (mg-Cl2 L(-1)) should be added when there was a high level of ammonia nitrogen and nitrite nitrogen in the reclaimed water. Therefore, 24-h chlorination without dechlorination or using only non-reductive quenching reagents (e.g. ammonium) for dechlorination and a total chlorine dose of 3× DOC + 8× ammonia nitrogen + 5× nitrite nitrogen (mg-Cl2 L(-1)) should be fulfilled for the AEAFP measurement. Moreover, the AEAFP (0.2-2.1 mg-TAM L(-1)) of the reclaimed water samples (n = 20) were further analyzed. The AEAFP was highly correlated to UV254 and the fluorescence volume in excitation emission matrix fluorescence spectrum which can be used as surrogates to indicate the level of the AEAFP and assess the precursors in reclaimed water.

Increase of cytotoxicity during wastewater chlorination: Impact factors and surrogates

Toxic and harmful disinfection byproducts (DBPs) were formed during wastewater chlorination. It was recently suggested that cytotoxicity to mammalian cells reflects risks posed by chlorinated wastewater. Here, ATP assays were performed to evaluate the cytotoxicity to mammalian cells. Chlorination significantly increased cytotoxicity of treated wastewater. Factors affecting cytotoxicity formation during wastewater chlorination were investigated. Quenching with sodium thiosulfate and ascorbic acid decreased the formed cytotoxicity, while ammonium kept the cytotoxicity stable. The chlorine dose required for the maximum cytotoxicity increase was dramatically affected by DOC and ammonia concentrations. The maximum cytotoxicity increase, defined as the cytotoxicity formation potential (CtFP), occurred when wastewater was treated for 48h with a chlorine dose of 2·DOC+11·NH3N+10 (mg-Cl2/L). During chlorination, the amounts of AOX formation was found to be significantly correlated with cytotoxicity formation when no DBPs were destroyed. AOX formation could be used as a surrogate to estimate cytotoxicity increase during wastewater chlorination. Besides, the CtFP of 14 treated wastewater samples was assessed ranged from 5.4-20.4mg-phenol/L. The CtFP could be estimated from UV254 of treated wastewater because CtFP and UV254 were strongly correlated.

Removal of fluorescence and ultraviolet absorbance of dissolved organic matter in reclaimed water by solar light

Storing reclaimed water in lakes is a widely used method of accommodating changes in the consumption of reclaimed water during wastewater reclamation and reuse. Solar light serves as an important function in degrading pollutants during storage, and its effect on dissolved organic matter (DOM) was investigated in this study. Solar light significantly decreased the UV254 absorbance and fluorescence (FLU) intensity of reclaimed water. However, its effect on the dissolved organic carbon (DOC) value of reclaimed water was very limited. The decrease in the UV254 absorbance intensity and FLU excitation-emission matrix regional integration volume (FLU volume) of reclaimed water during solar light irradiation was fit with pseudo-first order reaction kinetics. The decrease of UV254 absorbance was much slower than that of the FLU volume. Ultraviolet light in solar light had a key role in decreasing the UV254 absorbance and FLU intensity during solar light irradiation. The light fluence-based removal kinetic constants of the UV254 and FLU intensity were independent of light intensity. The peaks of the UV254 absorbance and FLU intensity with an apparent molecular weight (AMW) of 100Da to 2000Da decreased after solar irradiation, whereas the DOC value of the major peaks did not significantly change.

Formation and control of disinfection byproducts and toxicity during reclaimed water chlorination: A review

Chlorination is essential to the safety of reclaimed water; however, this process leads to concern regarding the formation of disinfection byproducts (DBPs) and toxicity. This study reviewed the formation and control strategies for DBPs and toxicity in reclaimed water during chlorination. Both regulated and emerging DBPs have been frequently detected in reclaimed water during chlorination at a higher level than those in drinking water, indicating they pose a greater risk to humans. Luminescent bacteria and Daphnia magna acute toxicity, anti-estrogenic activity and cytotoxicity generally increased after chlorination because of the formation of DBPs. Genotoxicity by umu-test and estrogenic activity were decreased after chlorination because of destruction of toxic chemicals. During chlorination, water quality significantly impacted changes in toxicity. Ammonium tended to attenuate toxicity changes by reacting with chlorine to form chloramine, while bromide tended to aggravate toxicity changes by forming hypobromous acid. During pretreatment by ozonation and coagulation, disinfection byproduct formation potential (DBPFP) and toxicity formation potential (TFP) occasionally increase, which is accompanied by DOC removal; thus, the decrease of DOC was limited to indicate the decrease of DBPFP and TFP. It is more important to eliminate the key fraction of precursors such as hydrophobic acid and hydrophilic neutrals. During chlorination, toxicities can increase with the increasing chlorine dose and contact time. To control the excessive toxicity formation, a relatively low chlorine dose and short contact time were required. Quenching chlorine residual with reductive reagents also effectively abated the formation of toxic compounds.

Transformation of DON in reclaimed water under solar light irradiation leads to decreased haloacetamide formation potential during chloramination

Reclaimed water is usually stored in rivers or lakes before subsequent use. In storage ecosystems, the natural process of solar light irradiation plays a key role in water quality, altering disinfection byproduct formation potential in later use. This study investigated changes in haloacetamide formation potential (HAcAm FP) during subsequent chloramination when reclaimed water was exposed to solar light irradiation. Significant decreases in HAcAm FP were observed for the solar light irradiated reclaimed water, with reductions of 27%-69% for different haloacetamides. Moreover, transformation of dissolved organic nitrogen (DON) to inorganic nitrogen occurred during irradiation. The application of 15N- labeled monochloramine indicated that the nitrogen source of the decreased HAcAms mainly originated from DON, rather than chloramine. Chloramination of the model compound l-asparagine after irradiation demonstrated that the decreased HAcAms could be attributed to the decrease in DON. After solar light irradiation, the brominated HAcAm FP in the presence of bromide was also reduced, while the bromine incorporation factor remained steady. Overall, this study revealed the contribution of natural processes in controlling HAcAm FP during subsequent chloramination, suggesting solar light irradiation is important to water purification during reclaimed water storage.

Exposure to solar light reduces cytotoxicity of sewage effluents to mammalian cells: Roles of reactive oxygen and nitrogen species

Sewage effluents can contain hundreds of toxic pollutants, making them a risk to humans when involved in drinking water. It is therefore important to evaluate the cytotoxicity of sewage effluents to mammalian cells. Solar light might influence the water quality of sewage effluents after their discharge into lakes or rivers, altering their cytotoxicity. In this study, natural solar light was found to lower the cytotoxicity of sewage effluents to Chinese hamster ovary (CHO) cells. Cytotoxicity of different samples decreased by 31%-65% after 12 h of simulated irradiation. Ultraviolet in sunlight was the major contributor to the cytotoxicity reduction. Aquatic reactive oxygen species (ROS), including singlet oxygen, superoxide anions, hydrogen peroxide, and hydroxyl radicals, were generated in the effluents under irradiation and they contributed to part of cytotoxicity reduction. Pollutants in sewage effluents induced cytotoxicity by simultaneously elevating the levels of intracellular ROS and intracellular reactive nitrogen species (RNS) in CHO cells. Solar light and the aquatic ROS formed under irradiation reduced the cytotoxicity because the transformed pollutants in sewage effluents increased lower intracellular ROS and RNS levels. These results help reveal the detoxification mechanism of sewage effluents in natural environment.

Electron donating capacity reduction of dissolved organic matter by solar irradiation reduces the cytotoxicity formation potential during wastewater chlorination

After treated wastewater is discharged into surface water for unplanned indirect potable reuse, solar irradiation transforms the dissolved organic matter (DOM), which would alter the formation of disinfection byproducts (DBPs) and change the cytotoxicity formation potential (CtFP) during post-chlorination in drinking water treatment plants. This study investigated the effects of solar irradiation on the CtFP and total organic halogen formation potential (TOXFP) of wastewater during post-chlorination. Exposure to natural sunlight decreased the formation potential of cytotoxicity to Chinese Hamster Ovary cells. Under 24 h simulated solar irradiation, CtFP and TOXFP decreased by more than 40%. X-ray photoelectron spectra and Fourier transformation infrared spectra suggested solar irradiation destroyed the key DBP precursors containing phenolic hydroxyl moieties (Ph-OH). The destruction of Ph-OH under solar irradiation was reflected by a decrease in the electron donating capacity (EDC) of DOM and the post-chlorination decreased the EDC further. Increasing the irradiation-consumed EDC abated the chlorine-consumed EDC, while the chlorine-consumed EDC was positively correlated to the CtFP and TOXFP by means of the electrophilic substitution-aromatic ring cleavage. Solar irradiation thus reduced the CtFP and TOXFP in wastewater during post-chlorination. This study revealed that solar irradiation decreased the risks of treated wastewater for unplanned indirect potable reuse and provided a strategy of controlling CtFP and TOXFP via reducing EDC of DOM in pretreatments.