Vertical-flow constructed wetlands as a sustainable on-site greywater treatment process for the decrease of micropollutant concentration in urban wastewater and integration to households' water services.

Micropollutant removal from effluent of conventional wastewater treatment has recently become one of the most discussed topics in the design and operation of wastewater treatment plants (WWTPs). This is due to the need to add a post-treatment step to the conventional processes to comply with stricter quality standards for effluents as outlined in the revised Urban Wastewater Treatment Directive (UWWTD). The adoption of on-site or decentralized greywater (GW) treatment in sustainable buildings using vertical-flow constructed wetlands (VFCWs) is a promising direction. It represents an interesting alternative for the removal of micropollutants at the source of pollution, such as personal care products (PCPs) and some pharmaceuticals which are mainly present in this wastewater fraction. Additionally, the treated greywater could be used in households' water services which do not require potable water quality, thus saving drinking water. In this context, this work compares the results of micropollutant removal from projects using VFCWs as a polishing step of WWTPs effluent, as a centralized solution, to the results from a decentralized GW treatment. The results show that VFCWs can remove the investigated micropollutants (Diclofenac and DEET) with an efficiency of >90 %, in both centralized and decentralized treatments. The admixture biochar from plant residues and from cellulose-toilet paper proved to be a promising substitute for the mineral zeolite when mixed with sand to remove PCPs from GW and, therefore, a circular economy concept can be applied to this technology.

Biochar from recovered cellulose as new admixture in constructed wetlands for micropollutant removal: A circular approach.

This study aimed to evaluate the suitability of biochar produced by pyrolysis from recovered wastewater cellulose and activated biologically as an admixture in Constructed Wetlands (CWs) when applied as a post-treatment step to remove micropollutants (MPs) from municipal wastewater effluent. Two planted vertical flow mesocosm CWs with cellulose-based admixtures of different origins (plant residue and recovered toilet paper) were fed with a municipal wastewater effluent representative for rural catchments. The results showed an average MPs elimination of 89.1 % for the activated biochar produced from recovered cellulose when 15 relevant compounds are considered and a reduction of the risk from compounds cocktail below the maximum acceptable level having diclofenac, carbamazepine, PFOS, ciprofloxacin and clarithromycin as main risk drivers (Risk Quotient > 1). The implementation of a circular approach to reduce MPs was finally conducted for the Blies catchment (Saarland region in Germany) characterized by low population density and small, sensitive water bodies. This approach demonstrates the feasibility of combining cellulose recovery with a fine sieve in large wastewater treatment plants (WWTPs) and providing biochar produced from recovered cellulose as an admixture to small WWTP where CW is an affordable solution for MP mitigation.

Fate of glyphosate and its metabolite AminoMethylPhosponic acid (AMPA) from point source through wastewater sludge and advanced treatment.

The fate of glyphosate and its metabolite AminoMethylPhosponic acid (AMPA) was followed at the catchment of the Sûre river, mainly characterized by small population density and small and medium-sized wastewater treatment plants (WWTPs). A high concentration of AMPA was found in water samples collected in inlet from different wastewater streams, the industry being the main contributor, while glyphosate resulted mainly in domestic origin. The two molecules were also monitored in the anaerobic digestion as in the supernatant produced after centrifugation (reject water). A total of 0.0713 and 2.24 g/d of glyphosate and AMPA respectively were regularly returned to the activated sludge tank (AST) indicating a 20% impact of the sludge management line on the global wastewater mass balance. Finally, the use of Constructed Wetlands (CWs) in Vertical Flow (VF) configuration was tested as a suitable technology to retain both glyphosate and AMPA (90 and up to 50% elimination respectively) and minimize their discharge into surface water.

Operation of a pilot-scale lipid accumulation technology employing parameters to select Microthrix parvicella for biodiesel production from wastewater.

Wastewater treatment plants (WWTPs) may play a crucial role in shifting to a zero-emission future by becoming more sustainable and contributing to the circular economy (CE). Recovered lipids from urban sewage can serve as a raw material for biofuel production contributing to a waste reduction, mitigation of natural resources depletion and reinforcing security and energy independence. A novel, pilot-scale lipid accumulation technology (LAT) employing parameters to select M. parvicella for the biofuel/biodiesel production was implemented on a side stream of an urban WWTP. The LAT proved its concept as the average amount of extracted lipids accumulated in the bioreactors was three-fold higher when compared to the lipids existing in activated sludge. The average transesterification of extracted lipids to biodiesel resulted in a 1.6 % yield, meaning that from 1 kg of dried sludge, 16 g of biodiesel could be formed. The biodiesel produced complies with European standard specifications (EN14214).

Assessing the impact of micropollutant mitigation measures using vertical flow constructed wetlands for municipal wastewater catchments in the greater region: a reference case for rural areas.

The present research aims at giving an approach to the issue of surface water contamination due to micropollutants in rural areas. The catchment of the Sûre river was selected as a reference case for the Greater Region, characterized mainly by settlements with low population density, small water bodies and small- to medium-sized wastewater treatment plants (WWTPs). For these WWTPs, conventional technical solutions for micropollutant elimination are not suitable; therefore, an adapted mitigation strategy is needed to prevent the impact of micropollutants, especially during the dry season. As a suitable alternative to more intensive technologies, Constructed Wetlands (CW) in Vertical Flow (VF) configuration have been successfully tested over a 1-year period and the elimination rate of 27 micropollutants was quantified. Emission reduction by VF was then considered in a static mass balance model that calculates the longitudinal concentration profile for the entire river catchment. The EmiSûre approach, which focuses on river quality (concentrations of pollutants) instead of emitted loads, effectively allowed simulation of adopted measures a priori and resulted in efficient support for decision-makers with WWTP upgrade scenarios.

Characterization of unconventional sand-based substrates for adsorption of micropollutants in nature-based systems.

The focus of this study is the characterization of unconventional sand-based substrates used in our previous project EmiSûre, (Interreg Greater Region (German federal states Rhineland-Palatinate and Saarland, the Grand Duchy of Luxembourg, regions Wallonia and Lorraine from Belgium and France, respectively), 2017-2021). The project aimed to develop and test alternative, nature-based technologies for the elimination of micropollutants (MPs) from municipal wastewater. For the characterization, two approaches were chosen. In the first approach, adsorption kinetics with a single compound allowed a perception of the adsorption capacity of the studied substrates compared to conventional substrates (granular activated carbons). This knowledge was completed by the second approach: an implementation of the studied substrates in packed-bed columns, which treated a mixture of 27 MPs in tap water for 10 months. Additionally, all three substrates (bentonite sand, sand with 15% activated biochar and sand with 15% zeolite) were characterized for physical and chemical properties, and the microbial potential of the activated and non-activated biochar was examined. From the studies, it is clear that the sand with an admixture of activated biochar is the most efficient sorbent in terms of single compound adsorption in batch (dye) and adsorption of 27 MPs on packed-bed columns. In contrast to the two other substrates, it shows long-term stable removal efficiencies. In the packed-bed columns, 18 out of 27 compounds were removed on average with high efficiency (80-99%), which is impressive, if we consider the variety of the compounds examined (pharmaceuticals, herbicides, pesticides, etc.) and their removal in conventional treatments. Additionally, adsorption models were created for the experimental data of all compounds adsorbed on the substrate with an admixture of activated biochar resulting in the best fit with the combined Langmuir-Freundlich model. These satisfying results suggest the application of the sand-based substrate with an admixture of activated biochar for further research and possibly upscale installations with the aim to offer and prove a reasonable and efficient alternative for MPs elimination from municipal wastewater.

Behaviour of 27 selected emerging contaminants in vertical flow constructed wetlands as post-treatment for municipal wastewater.

Six substrates (i.e. sand enriched with activated or non-activated biochar or zeolite in different ratios) were tested in Vertical Flow Constructed Wetlands (VFCWs) planted with Phragmites australis and Iris pseudacorus for the removal of 27 emerging contaminants from municipal wastewater. The laboratory investigation under controlled conditions (spiked constant concentrations in synthetic wastewater) lasted 357 days and proved VFCWs being able to provide excellent effluent quality in terms of both macro - and micropollutant elimination. Because overall removal efficiencies exceeded 90% in most of the cases, significant differences among the substrates were not detectable. For compounds with medium elimination (i.e. AMPA) the type of substrate seemed to play a strong role and the maximum amount of active ingredient adsorbed per amount of substrate has been quantified (i.e. 0.77 µg of AMPA per g of 30% biochar mixed with sand). Three of the most promising substrates from laboratory where thus selected to be tested under real conditions (fluctuation in concentration, variable temperature). As result, VFCWs with 15% activated biochar mixed with sand proved to be effective in the removal of 18 emerging contaminants and complying with national discharge standards for 4 selected compounds.

Removal of 27 micropollutants by selected wetland macrophytes in hydroponic conditions.

In this work, the primary focus is given on a mixture of 27 micropollutants (pharmaceuticals, pesticides, herbicides, fungicides and others) and its removal from aqueous solution by phytoremediation. Phytoremediation belongs to technologies, which are contributing on removal of micropollutants from wastewater in constructed wetlands. Constructed wetlands can be used as an additional step for elimination of micropollutants from municipal medium-sized wastewater treatment plants. To our knowledge, such a broad variety of micropollutants was never targeted for removal by phytoremediation before. In this work, we carry out experiments with 3 emergent macrophytes: Phragmites australis, Iris pseudacorus and Lythrum salicaria in hydroponic conditions. The selected plants are exposed to mixture of micropollutants in concentrations 1-14 mg/l for a time period of 30 days. The highest affinity for phytoremediation is detected at groups of fluorosurfactants (removal rate up to 30%), beta-blockers (removal rate up to 50%) and antibiotics (removal rate up to 90%). The leading capability for micropollutant uptake is detected at Lythrum salicaria, where 25 out of 27 compounds are removed with more than 20% efficiency. The results demonstrate well usefulness of this technology e.g. in an additional treatment step, because the mentioned groups of micropollutants are removed with comparable or even higher effectivity, than it is in case of conventional wastewater treatment plants.

Characterisation of class 3 integrons with oxacillinase gene cassettes in hospital sewage and sludge samples from France and Luxembourg.

In this study, antibiotic resistance class 3 integrons in Gram-negative bacteria isolated from hospital sewage and sludge and their genetic contents were characterised. Two samples of hospital effluent from France and Luxembourg and one sample of sludge from a wastewater treatment plant in France were collected in 2010 and 2011. Bacteria were cultured on selective agar plates and integrons were detected in colonies by quantitative PCR. Integron gene cassette arrays and their genetic environments were analysed by next-generation sequencing. Three class 3 integron-positive isolates were detected, including Acinetobacter johnsonii LIM75 (French hospital effluent), Aeromonas allosaccharophila LIM82 (sludge) and Citrobacter freundii LIM86 (Luxembourg hospital effluent). The gene cassettes were all implicated in antibiotic (aminoglycoside and ß-lactam) or antiseptic resistance. An oxacillinase gene cassette (blaOXA-10, blaOXA-368 or blaOXA-2) was found in each integron. All of the class 3 integrons were located on small mobilisable plasmids. This study highlights the role of class 3 integrons in the dissemination of clinically relevant antibiotic resistance genes, notably oxacillinase genes, in hospital effluent.

Tracer tests and uncertainty propagation to design monitoring setups in view of pharmaceutical mass flow analyses in sewer systems.

The development of a strategic approach to manage pollution of surface waters with pharmaceutical residues is in centre of interest in Europe. In this context a lack of reliable standard procedures for sampling and subsequent assessment of pharmaceutical mass flows in the water cycle has been identified. Authoritative assessment of relevant substance concentrations and flows is essential for environmental risk assessments and reliable efficiency analysis of measures to reduce or avoid emissions of drugs to water systems. Accordingly, a detailed preparation of monitoring campaigns including an accuracy check for the sampling configuration provides important information on the reliability of the gathered data. It finally supports data analysis and interpretation for evaluations of the efficiency of measures as well as for cost benefit assessments. The precision of mass flow balances is expected to be particularly weak when substances with high short-term variations and rare upstream emissions are considered. This is especially true for substance flow analysis in sewers close to source because of expectable highly dynamic flow conditions and emission patterns of pollutants. The case study presented here focusses on the verification of a monitoring campaign in a hospital sewer in Luxembourg. The results highlight the importance for a priori accuracy checks and provide a blueprint for well-designed monitoring campaigns of pharmaceutical trace pollutants on the one hand. On the other hand, the study provides evidence that the defined and applied continuous flow proportional sampling procedure enables a representative monitoring of short-term peak loads of the x-ray contrast media iobitridol close to source.

Comparative and integrative environmental assessment of advanced wastewater treatment processes based on an average removal of pharmaceuticals.

Pharmaceuticals are normally barely removed by conventional wastewater treatments. Advanced technologies as a post-treatment, could prevent these pollutants reaching the environment and could be included in a centralized treatment plant or, alternatively, at the primary point source, e.g. hospitals. In this study, the environmental impacts of different options, as a function of several advanced treatments as well as the centralized/decentralized implementation options, have been evaluated using Life Cycle Assessment (LCA) methodology. In previous publications, the characterization of the toxicity of pharmaceuticals within LCA suffers from high uncertainties. In our study, LCA was therefore only used to quantify the generated impacts (electricity, chemicals, etc.) of different treatment scenarios. These impacts are then weighted by the average removal rate of pharmaceuticals using a new Eco-efficiency Indicator EFI. This new way of comparing the scenarios shows significant advantages of upgrading a centralized plant with ozonation as the post-treatment. The decentralized treatment option reveals no significant improvement on the avoided environmental impact, due to the comparatively small pollutant load coming from the hospital and the uncertainties in the average removal of the decentralized scenarios. When comparing the post-treatment technologies, UV radiation has a lower performance than both ozonation and activated carbon adsorption.

Is it better to remove pharmaceuticals in decentralized or conventional wastewater treatment plants? A life cycle assessment comparison.

After ingestion, pharmaceuticals are excreted unchanged or metabolized. They subsequently arrive in conventional wastewater treatment plants and are then released into the environment, often without undergoing any degradation. Conventional treatment plants can be upgraded with post treatment, alternatively the removal of pharmaceuticals could be achieved directly at point sources. In the European project PILLS, several solutions for decentralized treatment of pharmaceuticals at hospitals were investigated at both pilot plant and full scale, and were then compared to conventional and upgraded centralized treatment plants using Life Cycle Assessment (LCA). Within the scope of the study, pharmaceuticals were found to have a comparatively minor environmental impact. As a consequence, an additional post treatment does not provide significant benefits. In the comparison of post treatment technologies, ozonation and activated carbon performed better than UV. These results suffer however from high uncertainties due to the assessment models of the toxicity of pharmaceuticals in LCA. Our results should therefore be interpreted with caution. LCA is a holistic approach and does not cover effects or issues on a local level, which may be highly relevant. We should therefore apply the precautionary ALARA principle (As Low As Reasonably Achievable) and not conclude that the effect of pharmaceuticals is negligible in the environment.