Although strictly anaerobic conditions prevail in several environmental compartments, up to now, biodegradation studies with emerging organic contaminants (EOCs), such as pharmaceuticals and personal ...care products, have mainly focused on aerobic conditions. One of the reasons probably is the assumption that the aerobic degradation is more energetically favorable than degradation under strictly anaerobic conditions. Certain aerobically recalcitrant contaminants, however, are biodegraded under strictly anaerobic conditions and little is known about the organisms and enzymatic processes involved in their degradation. This review provides a comprehensive survey of characteristic anaerobic biotransformation reactions for a variety of well-studied, structurally rather simple contaminants (SMOCs) bearing one or a few different functional groups/structural moieties. Furthermore it summarizes anaerobic degradation studies of more complex contaminants with several functional groups (CMCs), in soil, sediment and wastewater treatment. While strictly anaerobic conditions are able to promote the transformation of several aerobically persistent contaminants, the variety of observed reactions is limited, with reductive dehalogenations and the cleavage of ether bonds being the most prevalent. Thus, it becomes clear that the transferability of degradation mechanisms deduced from culture studies of SMOCs to predict the degradation of CMCs, such as EOCs, in environmental matrices is hampered due the more complex chemical structure bearing different functional groups, different environmental conditions (e.g. matrix, redox, pH), the microbial community (e.g. adaptation, competition) and the low concentrations typical for EOCs.
•Survey of characteristic anaerobic biotransformation reactions for classical contaminants.•Summary of anaerobic degradation studies on EOCs in soil, sediment and wastewater treatment.•Limited reactions observed for EOCs compared to classical contaminants.•Critical discussion of transferability of reactions from classical contaminants to EOCs.•Discussion of potential of anaerobic conditions for technical processes.
Conventional wastewater treatment plants are ineffective in removing a broad range of micropollutants, resulting in the release of these compounds into the aquatic environment, including natural ...drinking water resources. Ozonation is a suitable treatment process for micropollutant removal, although, currently, little is known about the formation, behavior, and removal of transformation products (TP) formed during ozonation. We investigated the elimination of 30 selected micropollutants (pharmaceuticals, X-ray contrast media, industrial chemicals, and TP) by biological treatment coupled with ozonation and, subsequently, in parallel with two biological filters (BF) or granular activated carbon (GAC) filters. The selected micropollutants were removed to very different extents during the conventional biological wastewater treatment process. Ozonation (specific ozone consumption: 0.87 ± 0.29 gO3 gDOC−1, hydraulic retention time: 17 ± 3 min) eliminated a large number of the investigated micropollutants. Although 11 micropollutants could still be detected after ozonation, most of these were eliminated in subsequent GAC filtration at bed volumes (BV) of approximately 25,000 m3 m−3. In contrast, no additional removal of micropollutants was achieved in the BF. Ozonation of the analgesic tramadol led to the formation of tramadol-N-oxide that is effectively eliminated by GAC filters, but not by BF. For the antiviral drug acyclovir, the formation of carboxy-acyclovir was observed during activated sludge treatment, with an average concentration of 3.4 ± 1.4 μg L−1 detected in effluent samples. Subsequent ozonation resulted in the complete elimination of carboxy-acyclovir and led to the formation of N-(4-carbamoyl-2-imino-5-oxo imidazolidin)-formamido-N-methoxyacetetic acid (COFA; average concentration: 2.6 ± 1.0 μg L−1). Neither the BF nor the GAC filters were able to remove COFA. These results highlight the importance of considering TP in the evaluation of advanced wastewater treatment processes. The results further indicate that post-treatment of ozonated wastewater with GAC filtration seems to be more suitable than BF, due to the sorption of formed TP to the activated carbon.
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•Advanced wastewater treatment with ozonation and subsequent biofilters or GAC filters was investigated.•Transformation products were formed during conventional wastewater treatment and ozonation.•Biofilters were not capable to eliminate the transformation products tramadol-N-oxide and COFA.•GAC Filters eliminate tramadol-N-oxide but COFA was detected in nearly the same concentration.•Remaining micropollutants after ozonation were mostly eliminated by subsequent GAC filters but not by biofilters.
Plastics are known sources of chemical exposure and few, prominent plastic-associated chemicals, such as bisphenol A and phthalates, have been thoroughly studied. However, a comprehensive ...characterization of the complex chemical mixtures present in plastics is missing. In this study, we benchmark plastic consumer products, covering eight major polymer types, according to their toxicological and chemical signatures using in vitro bioassays and nontarget high-resolution mass spectrometry. Most (74%) of the 34 plastic extracts contained chemicals triggering at least one end point, including baseline toxicity (62%), oxidative stress (41%), cytotoxicity (32%), estrogenicity (12%), and antiandrogenicity (27%). In total, we detected 1411 features, tentatively identified 260, including monomers, additives, and nonintentionally added substances, and prioritized 27 chemicals. Extracts of polyvinyl chloride (PVC) and polyurethane (PUR) induced the highest toxicity, whereas polyethylene terephthalate (PET) and high-density polyethylene (HDPE) caused no or low toxicity. High baseline toxicity was detected in all “bioplastics” made of polylactic acid (PLA). The toxicities of low-density polyethylene (LDPE), polystyrene (PS), and polypropylene (PP) varied. Our study demonstrates that consumer plastics contain compounds that are toxic in vitro but remain largely unidentified. Since the risk of unknown compounds cannot be assessed, this poses a challenge to manufacturers, public health authorities, and researchers alike. However, we also demonstrate that products not inducing toxicity are already on the market.
Removal of organic micropollutants was investigated in 15 diverse biological reactors through short and long-term experiments. Short-term batch experiments were performed with activated sludge from ...three parallel sequencing batch reactors (25, 40, and 80 d solid retention time, SRT) fed with synthetic wastewater without micropollutants for one year. Despite the minimal micropollutant exposure, the synthetic wastewater sludges were able to degrade several micropollutants present in municipal wastewater. The degradation occurred immediately after spiking (1–5 μg/L), showed no strong or systematic correlation to the sludge age, and proceeded at rates comparable to those of municipal wastewater sludges. Thus, the results from the batch experiments indicate that degradation of organic micropollutants in biological wastewater treatment is quite insensitive to SRT increases from 25 to 80 days, and not necessarily induced by exposure to micropollutants. Long-term experiments with municipal wastewater were performed to assess the potential for extended biological micropollutant removal under different redox conditions and substrate concentrations (carbon and nitrogen). A total of 31 organic micropollutants were monitored through influent-effluent sampling of twelve municipal wastewater reactors. In accordance with the results from the sludges grown on synthetic wastewater, several compounds such as bezafibrate, atenolol and acyclovir were significantly removed in the activated sludge processes fed with municipal wastewater. Complementary removal of two compounds, diuron and diclofenac, was achieved in an oxic biofilm treatment. A few aerobically persistent micropollutants such as venlafaxine, diatrizoate and tramadol were removed under anaerobic conditions, but a large number of micropollutants persisted in all biological treatments. Collectively, these results indicate that certain improvements in biological micropollutant removal can be achieved by combining different aerobic and anaerobic treatments, but that these improvements are restricted to a limited number of compounds.
•Micropollutant removal in 15 different reactors with >10 years of total operation.•Micropollutant removal under different substrate availabilities and redox.•Immediate micropollutant degradation without prior adaptation.•Advanced biological treatment improved removal for 25% of the compounds studied.•Half of the micropollutants could not be effectively targeted biologically.
The knowledge we have gained in recent years on the presence and effects of compounds discharged by wastewater treatment plants (WWTPs) brings us to a point where we must question the appropriateness ...of current water quality evaluation methodologies. An increasing number of anthropogenic chemicals is detected in treated wastewater and there is increasing evidence of adverse environmental effects related to WWTP discharges. It has thus become clear that new strategies are needed to assess overall quality of conventional and advanced treated wastewaters. There is an urgent need for multidisciplinary approaches combining expertise from engineering, analytical and environmental chemistry, (eco)toxicology, and microbiology. This review summarizes the current approaches used to assess treated wastewater quality from the chemical and ecotoxicological perspective. Discussed chemical approaches include target, non-target and suspect analysis, sum parameters, identification and monitoring of transformation products, computational modeling as well as effect directed analysis and toxicity identification evaluation. The discussed ecotoxicological methodologies encompass in vitro testing (cytotoxicity, genotoxicity, mutagenicity, endocrine disruption, adaptive stress response activation, toxicogenomics) and in vivo tests (single and multi species, biomonitoring). We critically discuss the benefits and limitations of the different methodologies reviewed. Additionally, we provide an overview of the current state of research regarding the chemical and ecotoxicological evaluation of conventional as well as the most widely used advanced wastewater treatment technologies, i.e., ozonation, advanced oxidation processes, chlorination, activated carbon, and membrane filtration. In particular, possible directions for future research activities in this area are provided.
•Review of chemical and ecotoxicological methods to assess wastewater quality.•Critical assessment of methods including benefits and limitations.•Critical evaluation of conventional and advanced treatment technologies.•Demand for multidisciplinary assessment approaches and future research identified.
The fate of five antiviral drugs (abacavir, emtricitabine, ganciclovir, lamivudine and zidovudine) was investigated in biological wastewater treatment. Investigations of degradation kinetics were ...accompanied by the elucidation of formed transformation products (TPs) using activated sludge lab experiments and subsequent LC-HRMS analysis. Degradation rate constants ranged between 0.46 L d−1 gSS−1 (zidovudine) and 55.8 L d−1 gSS−1 (abacavir). Despite these differences of the degradation kinetics, the same main biotransformation reaction was observed for all five compounds: oxidation of the terminal hydroxyl-moiety to the corresponding carboxylic acid (formation of carboxy-TPs). In addition, the oxidation of thioether moieties to sulfoxides was observed for emtricitabine and lamivudine.
Antiviral drugs were detected in influents of municipal wastewater treatment plants (WWTPs) with concentrations up to 980 ng L−1 (emtricitabine), while in WWTP effluents mainly the TPs were found with concentration levels up to 1320 ng L−1 (carboxy-abacavir). Except of zidovudine none of the original antiviral drugs were detected in German rivers and streams, whereas the concentrations of the TPs ranged from 16 ng L−1 for carboxy-lamivudine up to 750 ng L−1 for carboxy-acyclovir. These concentrations indicate an appreciable portion from WWTP effluents present in rivers and streams, as well as the high environmental persistence of the carboxy-TPs. As a result three of the carboxylic TPs were detected in finished drinking water.
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•New biological transformation products of antiviral drugs were identified to be formed in WWTPs.•Carboxy-TPs were found in rivers, streams and drinking water.•Transformation products can be removed by ozonation and partly by powdered activated carbon.
The implementation of autotrophic anaerobic ammonium oxidation processes for the removal of nitrogen from municipal wastewater (known as “mainstream anammox”) bears the potential to bring wastewater ...treatment plants close to energy autarky. The aim of the present work was to assess the long-term stability of partial nitritation/anammox (PN/A) processes operating at low temperatures and their reliability in meeting nitrogen concentrations in the range of typical discharge limits below 2 mgNH4-N·L−1 and 10 mgNtot·L−1. Two main 12-L sequencing batch reactors were operated in parallel for PN/A on aerobically pre-treated municipal wastewater (21 ± 5 mgNH4-N·L−1 and residual 69 ± 19 mgCODtot·L−1) for more than one year, including over 5 months at 15 °C. The two systems consisted of a moving bed biofilm reactor (MBBR) and a hybrid MBBR (H-MBBR) with flocculent biomass. Operation at limiting oxygen concentrations (0.15–0.18 mgO2·L−1) allowed stable suppression of the activity of nitrite-oxidizing bacteria at 15 °C with a production of nitrate over ammonium consumed as low as 16% in the MBBR. Promising nitrogen removal rates of 20–40 mgN·L−1·d−1 were maintained at hydraulic retention times of 14 h. Stable ammonium and total nitrogen removal efficiencies over 90% and 70% respectively were achieved. Both reactors reached average concentrations of total nitrogen below 10 mgN·L−1 in their effluents, even down to 6 mgN·L−1 for the MBBR, with an ammonium concentration of 2 mgN·L−1 (set as operational threshold to stop aeration). Furthermore, the two PN/A systems performed almost identically with respect to the biological removal of organic micropollutants and, importantly, to a similar extent as conventional treatments. A sudden temperature drop to 11 °C resulted in significant suppression of anammox activity, although this was rapidly recovered after the temperature was increased back to 15 °C. Analyses of 16S rRNA gene-targeted amplicon sequencing revealed that the anammox guild of the bacterial communities of the two systems was composed of the genus “Candidatus Brocadia”. The potential of PN/A systems to compete with conventional treatments for biological nutrients removal both in terms of removal rates and overall effluent quality was proven.
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•Stable partial nitritation/anammox of aerobically pre-treated municipal wastewater at 15 °C.•Effluent ammonia and total nitrogen concentrations meet current discharge limits.•Successful NOB activity suppression at low dissolved oxygen concentrations (0.15–0.18 mgO2/L).•Micropollutants removal comparable to conventional biological treatments.•Reversible but dramatic anammox activity suppression during prolonged operation at 11 °C.
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