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An underemphasized aspect of sampling strategies in effect-based in vitro testing is to determine suitable collection and preparation techniques. In the current study, the impact of sample acidification on bioactivities was assessed using in vitro bioassays for hormone receptor-mediated effects (estrogen receptor [ER] and androgen receptor [AR]) and the oxidative stress response (Nrf2 activity). Sampling was conducted at a recently upgraded Swedish wastewater treatment plant. Future plans for the treated wastewater include reuse for irrigation or as a potential drinking water source. In the AR and Nrf2 assays, acidification decreased bioactivities in the wastewater influent sample extracts, whereas acidification increased bioactivities following further treatment (disc filtration). In the ER assay, acidification had no impact on the observed bioactivities in the sample extracts. A secondary objective of the study was to assess the stability of the sample extracts over time. Lower activities were detected in the ER and AR assays in all extracts after storage for approximately 1 year. Nrf2 activities did not decrease over time, but rather increased in some of the acidified sample extracts. Overall, the findings suggest that sampling strategies involving acidification may need to be tailored depending on the selected bioassay(s) and the type of wastewater treatments being assessed.

Drinking water producers have a far-reaching responsibility to provide safe, clean and wholesome drinking water, using water resources possibly effected by the thousands of chemicals used in societies’ daily life. This study has monitored chemical hazards in drinking water from source to tap, using effect-based methods. The study was conducted at a Swedish drinking water treatment plant sourcing lake water and aimed to investigate potential seasonal variations in both the raw water and water after different treatment steps. Furthermore, a granular activated carbon (GAC) pilot facility was evaluated. Samples were analyzed for estrogenicity, androgenicity, aryl hydrocarbon receptor (AhR) activity, oxidative stress (Nrf2) response and genotoxicity (micronucleus formation). We observed seasonal differences in oxidative stress and genotoxic effects in both raw and drinking water with higher activities during the late fall of each year. The removal efficiency for both oxidative stress and genotoxicity was limited in the full-scale treatment process and occasionally the genotoxicity was also detected in outgoing drinking water from the treatment plant and in samples collected at consumers tap on the distribution network. AhR activity was present in all raw water samples and the removal was limited. Estrogenic activities were observed in most of the raw water samples but in contrast to the other parameters estrogenicity was effectively reduced by the full-scale conventional treatment. The GAC pilot treatment was generally more efficient than the full-scale conventional treatment in removing all observed bioactivities and could be a viable complement to the current treatment to assure drinking water free from genotoxic compounds. Genotoxic activities in drinking water was observed while all currently regulated chemical parameters were fulfilled. This highlights the need for effect-based monitoring in efforts to ensure the chemical safety of drinking water, as target chemical analysis of single compounds will overlook both unknown hazardous compounds as well as potential mixture effects. Graphical Abstract

BackgroundBioanalytical tools have been shown to be useful in drinking water quality assessments. Here, we applied a panel of in vitro bioassays to assess the treatment efficiency of two pilot-scale treatments: ozonation and granular activated carbon (GAC) filtration at a drinking water treatment plant (DWTP). The pilot-scale systems were studied alongside a full-scale treatment process consisting of biological activated carbon (BAC) filtration, UV disinfection, and monochloramine dosing. Both systems were fed the same raw water treated with coagulation/flocculation/sedimentation and sand filtration. The endpoints studied were oxidative stress (Nrf2 activity), genotoxicity (micronuclei formations), aryl hydrocarbon receptor (AhR) activation, as well as estrogen receptor (ER) and androgen receptor (AR) activity.ResultsNrf2, AhR, and ER activities and genotoxic effects were detected in the incoming raw water and variability was observed between the sampling events. Compared to most of the samples taken from the full-scale treatment system, lower Nrf2, AhR, and ER bioactivities as well as genotoxicity were observed in all samples from the pilot-scale systems across all sampling events. The most pronounced treatment effect was a 12-fold reduction in Nrf2 activity and a sixfold decrease in micronuclei formations following ozonation alone. GAC filtration alone resulted in sevenfold and fivefold reductions in Nrf2 activity and genotoxicity, respectively, in the same sampling event. Higher bioactivities were detected in most samples from the full-scale system suggesting a lack of treatment effect. No androgenic nor anti-androgenic activities were observed in any sample across all sampling events.ConclusionsUsing effect-based methods, we have shown the presence of bioactive chemicals in the raw water used for drinking water production, including oxidative stress, AhR and ER activities as well as genotoxicity. The currently used treatment technologies were unable to fully remove the observed bioactivities. Ozonation and GAC filtration showed a high treatment efficiency and were able to consistently remove the bioactivities observed in the incoming water. This is important knowledge for the optimization of existing drinking water treatment designs and the utilization of alternative treatment technologies.

Granulated active carbon (GAC) is commonly used as a chemical barrier for the removal of organic micropollutants (OMPs) in drinking water treatment plants (DWTPs). However, little is known about the impact of dissolved organic carbon (DOC) and its long-term performance with regard to OMP removal efficiency. This study examined the performance of two GAC types (Norit 830W and Filtrasorb 400) in the removal of OMPs and DOC from natural lake water, in pilot-scale and full-scale tests run for almost one year. Potential early warning indicators of the exhaustion of GAC sorption capacity were also evaluated. The seven OMPs investigated (carbamazepine, lamotrigine, cetirizine, fexofenadine, oxazepam, fluconazole and N,N-diethyl-meta-toluamide (DEET)) all showed decreasing removal efficiencies after ~20,000 bed volumes (BV) in the pilot-scale Norit 830W and Filtrasorb 400 columns. However, columns with an 18-min empty bed contact time (EBCT) showed better performances than columns with 6-min EBCT. DEET was the OMP adsorbed most weakly. We found that DOC concentrations, methylene blue sorption kinetics, UV and fluorescence did not sufficiently explain the OMP breakthrough in the GAC columns. We concluded that carbamazepine, lamotrigine and fexofenadine can be used as indicators of decreasing GAC adsorption performance, due to their later breakthrough. Based on the results, UV and fluorescence removal could be used for the early detection of declining DOC removal, and online solid-phase extraction (SPE)–liquid chromatography–tandem mass spectrometry (SPE-LC-MS/MS) could be used for the early detection of OMPs in drinking water.

Granulated active carbon (GAC) is commonly used as a chemical barrier for the removal of organic micropollutants (OMPs) in drinking water treatment plants (DWTPs). However, little is known about the impact of dissolved organic carbon (DOC) and its long-term performance with regard to OMP removal efficiency. This study examined the performance of two GAC types (Norit 830W and Filtrasorb 400) in the removal of OMPs and DOC from natural lake water, in pilot-scale and full-scale tests run for almost one year. Potential early warning indicators of the exhaustion of GAC sorption capacity were also evaluated. The seven OMPs investigated (carbamazepine, lamotrigine, cetirizine, fexofenadine, oxazepam, fluconazole and N,N-diethyl-meta-toluamide (DEET)) all showed decreasing removal efficiencies after -20,000 bed volumes (BV) in the pilot-scale Norit 830W and Filtrasorb 400 columns. However, columns with an 18-min empty bed contact time (EBCT) showed better performances than columns with 6-min EBCT. DEET was the OMP adsorbed most weakly. We found that DOC concentrations, methylene blue sorption kinetics, UV and fluorescence did not sufficiently explain the OMP breakthrough in the GAC columns. We concluded that carbamazepine, lamotrigine and fexofenadine can be used as indicators of decreasing GAC adsorption performance, due to their later breakthrough. Based on the results, UV and fluorescence removal could be used for the early detection of declining DOC removal, and online solid-phase extraction (SPE)-liquid chromatography-tandem mass spectrometry (SPE-LC-MS/MS) could be used for the early detection of OMPs in drinking water. Keywords: granulated active carbon; pharmaceuticals; removal efficiency; breakthrough; methylene blue