Suchergebnisse

Contamination of soils with organic pollutants is an increasing global problem, so novel soil remediation techniques are urgently needed. One such technique is electrokinetic remediation, in which an electric field is applied over the soil to extract contaminants. Previous evaluations of the technique have been limited to a few specific compounds. In this study, we integrated the latest advances in high-resolution mass spectrometry (HRMS) to identify molecular fingerprints, and used the results to improve the mechanistic understanding necessary for successful remediation. A laboratory-scale 0.38 mA cm−2 electrodialytic treatment was applied for 21 days to a contaminated soil from a firefighter training facility in Sweden. Non-target analysis allowed generic evaluation of changes in the soil organic fraction by tentatively determining the elemental composition of compounds present. The results showed that smaller oxygen-rich molecules were significantly transported to the anode by electromigration, while larger hydrogen-saturated molecules were transported to the cathode by electroosmotic flow. Wide suspect screening with >3000 per- and polyfluoroalkyl substances (PFASs) tentatively identified seven new PFASs in the test soil, including perfluoroheptanesulfonic acid (PFHpS), and PFASs with butoxy, ethoxy, ethanol, and ethylcyclohexanesulfonate functional groups ; This work was supported by the project PFAS-PURE from VINNOVA, Sweden (2015-03561). Pablo Gago-Ferrero acknowledges the European Union's Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement Smart-Workflow No 747698

Contamination of soils with organic pollutants is an increasing global problem, so novel soil remediation techniques are urgently needed. One such technique is electrokinetic remediation, in which an electric field is applied over the soil to extract contaminants. Previous evaluations of the technique have been limited to a few specific compounds. In this study, we integrated the latest advances in high-resolution mass spectrometry (HRMS) to identify molecular fingerprints, and used the results to improve the mechanistic understanding necessary for successful remediation. A laboratory-scale 0.38 mA cm−2 electrodialytic treatment was applied for 21 days to a contaminated soil from a firefighter training facility in Sweden. Non-target analysis allowed generic evaluation of changes in the soil organic fraction by tentatively determining the elemental composition of compounds present. The results showed that smaller oxygen-rich molecules were significantly transported to the anode by electromigration, while larger hydrogen-saturated molecules were transported to the cathode by electroosmotic flow. Wide suspect screening with >3000 per- and polyfluoroalkyl substances (PFASs) tentatively identified seven new PFASs in the test soil, including perfluoroheptanesulfonic acid (PFHpS), and PFASs with butoxy, ethoxy, ethanol, and ethylcyclohexanesulfonate functional groups. ; This work was supported by the project PFAS-PURE from VINNOVA, Sweden (2015-03561). Pablo Gago-Ferrero acknowledges the European Union's Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement Smart-Workflow No 747698. The authors acknowledge the Trace Analysis and Mass Spectrometry Group (TrAMS of the University of Athens) for support with chemometric tools, and the Danish Technical University (DTU BYG) for experimental support. ; Peer reviewed

In order to understand and minimize the formation of halogenated disinfection by-products (DBPs), it is important to investigate how dissolved organic matter (DOM) contributes to their generation. In the present study, we analysed the DOM profile of water samples from the Barcelona catchment area by high resolution mass spectrometry (HRMS) and we studied the changes after chlorination. Chlorination produced significant changes in the DOM, decreased the average m/z and Kendrick mass defect (KMD) of their spectra and decreased the number and abundance of lignin-like features. The Van Krevelen (VK) fingerprint exhibited several noticeable changes, including the appearance of highly oxidized peaks in the tannin-like region (average O/C, 0.78 ± 0.08), the appearance of features with low H/C and the disappearance of more than half of the lipids-like features. Up to 657 halogenated peaks were generated during sample chlorination, most of which in the condensed hydrocarbons-like and the lignin-like region of the VK diagram. Around 200 features were found to be strongly correlated (ρ ≥ 0.795) to the formation potential of trihalomethanes (THMs) and 5 were correlated with the formation potential of haloacetonitrile (HANs). They all were plotted in the lignin fraction of the VK diagram, but both groups of features exhibited different nitrogen content: those features related to HANs FP had at least one nitrogen atoms in their structures, whilst those related to THMs did not. ; This project was funded by the Spanish Ministry of Science,Innovation and Universities, AEI-MICIU, and the European Fund forRegional Development under the National Program for Research Aimed at the Challenges of Society, through the project NDMA_Predict (CTM 2017-85335-R); and by the European Union's Horizon2020 Research and Innovation Programme, through the MANTEL-ITN Project (Grant No: 722518). The authors thank Generalitat deCatalunya through Consolidated Research Group ENV 2017 SGR1124 and Tech 2017 SGR 1318. ICRA researchers thank funding ...

Comunicació de congrés presentada a: 16 th International Conference on Environmental Science and Technology, celebrat a l'Illa de Rodes (Grecia), del 4 a 7 de setembre de 2019 ; This work aims at integrating the last advances in high resolution mass spectrometry (HRMS) and statistical analysis of data to develop and optimize a smart methodology (workflow) for the assessment of the performance of innovative water treatments using different technological approaches based on advanced oxidation processes with UV-254nm: (i) UV/K2S2O8, where oxidation takes place mainly following the initial formation of sulfate radicals, (ii) UV/KHSO5, where oxidation begins with the formation of both sulfate and hydroxyl radicals and (iii) UV/H2O2, when only the formation of hydroxyl radicals takes place initially. Experiments were carried out using secondary effluent from a local wastewater treatment plant. The developed workflow allows the evaluation of the treatments in terms of overall oxidation through the careful study of Van Krevelen diagrams, where all the masses of the HRMS chromatograms are considered. The potential formation of transformation products with sulfur due to the sulfate radicals was also evaluated using statistical tools based on the isotopic pattern and accurate mass. Finally, the behavior of a large number of micropollutants with a wide range of physicochemical properties was studied using suspect screening strategies ; This project has received funding from the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement SMARTWORKFLOW (747698), the Spanish Ministry of Science and Innovation (grant number CTQ2015-69832-C4), and the Economy and Knowledge Department of the Catalan Government (Consolidated Research Group program: ICRATECH - 2017 SGR 1318 and ICRA-ENV - 2017 SGR 01124)

Contaminants of emerging concern (CECs) are widespread in the water cycle. Their levels in disinfected waters are usually low, as they may transform into CEC disinfection byproducts (DBPs) during disinfection processes or partially removed in previous water treatment steps. The occurrence of CEC DBPs in real waters has been scarcely addressed, although their presence may be of relevance in water circular economy scenarios, and thus deserves further study in water regeneration systems. In this work, a database of CEC DBPs (n=1338) after chlorination was generated and is ready to use in future screening studies to assess the relevance of these chemicals in contaminat mixtures. Moreover, the transformation of CECs during chlorination, their main reaction pathways with chlorine, and current knowledge gaps were critically reviewed. ; CP acknowledges support from Fundación General del CSIC through the ComFuturo Programme (2nd edition). This work was supported by the Government of Catalonia (Consolidated Research Groups 2017 SGR 01404), and the "Agencia Estatal de Investigación" from the Spanish Ministry of Science and Innovation (MEDISTRAES III, PID2019-110212RB-C22) and the IDAEA-CSIC, a Centre of Excellence Severo Ochoa (CEX2018-000794-S). CP acknowledges support from the Swedish University of Agricultural Sciences through the August T Larsson Guest Researcher Programme. We would also like to acknowledge the personnel from the WWTPs that kindly assisted in water sample collection. ; Peer reviewed

While the extent of pharmaceutical consumption within a society/community is of high relevance to its health, economy and general wellbeing, this data is often not readily available. Herein, we strengthen a wastewater–based epidemiology (WBE) approach as a way to track the consumption of pharmaceuticals within the sampled community. This method is less laborious than established questionnaire or databases approaches and allows a higher temporal and spatial resolution. The WBE approach was conducted by sampling influent wastewater from two wastewater treatment plants of different size. A total of 39 targeted compounds were quantified by liquid chromatography coupled with tandem mass spectrometry. The number of prescriptions and the defined daily doses for each prescription was obtained from the reference database of The Catalan Health System to validate the wastewater-based approach. The wastewater sampling and the data inquiry were both executed during the same period (October 2019) and standardised for comparison to treatments per 1,000 inhabitants per day. The back-calculation parameters were improved from previous studies by including the faecal excretion rate of the pharmaceuticals. For prescription only pharmaceuticals, where prescription numbers are expected to be a good estimate of consumption, our WBE approach agreed with 27 out of 32 (<0.7 order of magnitude). Common over-the-counter pharmaceuticals such as acetaminophen, ibuprofen and naproxen showed much higher values for treatments per day per 1,000 inhabitant in wastewater than prescribed, reflecting the usefulness of WBE in obtaining an estimate of the total consumption i.e. with and without a prescription ; The study presents results from the SCOREwater project, which has received funding from the European Union's Horizon 2020 Research and Innovation Programme under grant agreement no 820751. Lluís Corominas and Sara Rodriguez-Mozaz acknowledge the Ministry of Economy and competitiveness for their Ramon and Cajal grants and the corresponding I3 ...

This study presents the development and validation of a comprehensive quantitative target methodology for the analysis of 2316 emerging pollutants in water based on Ultra-Performance Liquid Chromatography Quadrupole-Time-Of-Flight Mass Spectrometry (UPLC-Q-ToF-HRMS/MS). Target compounds include pesticides, pharmaceuticals, drugs of abuse, industrial chemicals, doping compounds, surfactants and transformation products, among others. The method was validated for 195 analytes, chosen to be representative of the chemical space of the target list, enabling the assessment of the performance of the method. The method involves a generic sample preparation based on mixed mode solid phase extraction, a UPLC-QTOF-MS/MS screening method using Data Independent Acquisition (DIA) mode, which provides MS and MS/MS spectra simultaneously and an elaborate strong post-acquisition evaluation of the data. The processing method was optimized to provide a successful identification rate >95 % and to minimize the number of false positive results (< 5 %). Decision limit (CCα) and detection capability (CCβ) were also introduced in the validation scheme to provide more realistic metrics on the performance of a HRMS-based wide-scope screening method. A new system of identification points (IPs) based on the one described in the Commission Decision 2002/657/EC was applied to communicate the confidence level in the identification of the analytes. This system considers retention time, mass accuracy, isotopic fit and fragmentation; taking full advantage of the capacities of the HRMS instruments. Finally, 398 contaminants were detected and quantified in real wastewater ; This project was implemented under the Operational Program "Education and Lifelong Learning" and funded by the European Union (European Social Fund) and Greek National Resources – ARISTEIA 624 (TREMEPOL project). Pablo Gago-Ferrero acknowledges the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement Smart-Workflow ...

Abstract
Background
Prioritisation of chemical pollutants is a major challenge for environmental managers and decision-makers alike, which is essential to help focus the limited resources available for monitoring and mitigation actions on the most relevant chemicals. This study extends the original NORMAN prioritisation scheme beyond target chemicals, presenting the integration of semi-quantitative data from retrospective suspect screening and expansion of existing exposure and risk indicators. The scheme utilises data retrieved automatically from the NORMAN Database System (NDS), including candidate substances for prioritisation, target and suspect screening data, ecotoxicological effect data, physico-chemical data and other properties. Two complementary workflows using target and suspect screening monitoring data are applied to first group the substances into six action categories and then rank the substances using exposure, hazard and risk indicators. The results from the 'target' and 'suspect screening' workflows can then be combined as multiple lines of evidence to support decision-making on regulatory and research actions.

Results
As a proof-of-concept, the new scheme was applied to a combined dataset of target and suspect screening data. To this end, > 65,000 substances on the NDS, of which 2579 substances supported by target wastewater monitoring data, were retrospectively screened in 84 effluent wastewater samples, totalling > 11 million data points. The final prioritisation results identified 677 substances as high priority for further actions, 7455 as medium priority and 326 with potentially lower priority for actions. Among the remaining substances, ca. 37,000 substances should be considered of medium priority with uncertainty, while it was not possible to conclude for 19,000 substances due to insufficient information from target monitoring and uncertainty in the identification from suspect screening. A high degree of agreement was observed between the categories assigned via target analysis and suspect screening-based prioritisation. Suspect screening was a valuable complementary approach to target analysis, helping to prioritise thousands of substances that are insufficiently investigated in current monitoring programmes.

Conclusions
This updated prioritisation workflow responds to the increasing use of suspect screening techniques. It can be adapted to different environmental compartments and can support regulatory obligations, including the identification of specific pollutants in river basins and the marine environments, as well as the confirmation of environmental occurrence levels predicted by modelling tools.

Graphical Abstract

AbstractIncreasing production and use of chemicals and awareness of their impact on ecosystems and humans has led to large interest for broadening the knowledge on the chemical status of the environment and human health by suspect and non-target screening (NTS). To facilitate effective implementation of NTS in scientific, commercial and governmental laboratories, as well as acceptance by managers, regulators and risk assessors, more harmonisation in NTS is required. To address this, NORMAN Association members involved in NTS activities have prepared this guidance document, based on the current state of knowledge. The document is intended to provide guidance on performing high quality NTS studies and data interpretation while increasing awareness of the promise but also pitfalls and challenges associated with these techniques. Guidance is provided for all steps; from sampling and sample preparation to analysis by chromatography (liquid and gas—LC and GC) coupled via various ionisation techniques to high-resolution tandem mass spectrometry (HRMS/MS), through to data evaluation and reporting in the context of NTS. Although most experience within the NORMAN network still involves water analysis of polar compounds using LC–HRMS/MS, other matrices (sediment, soil, biota, dust, air) and instrumentation (GC, ion mobility) are covered, reflecting the rapid development and extension of the field. Due to the ongoing developments, the different questions addressed with NTS and manifold techniques in use, NORMAN members feel that no standard operation process can be provided at this stage. However, appropriate analytical methods, data processing techniques and databases commonly compiled in NTS workflows are introduced, their limitations are discussed and recommendations for different cases are provided. Proper quality assurance, quantification without reference standards and reporting results with clear confidence of identification assignment complete the guidance together with a glossary of definitions. The NORMAN community greatly supports the sharing of experiences and data via open science and hopes that this guideline supports this effort.

Abstract
Background
The NORMAN Association (https://www.norman-network.com/) initiated the NORMAN Suspect List Exchange (NORMAN-SLE; https://www.norman-network.com/nds/SLE/) in 2015, following the NORMAN collaborative trial on non-target screening of environmental water samples by mass spectrometry. Since then, this exchange of information on chemicals that are expected to occur in the environment, along with the accompanying expert knowledge and references, has become a valuable knowledge base for "suspect screening" lists. The NORMAN-SLE now serves as a FAIR (Findable, Accessible, Interoperable, Reusable) chemical information resource worldwide.

Results
The NORMAN-SLE contains 99 separate suspect list collections (as of May 2022) from over 70 contributors around the world, totalling over 100,000 unique substances. The substance classes include per- and polyfluoroalkyl substances (PFAS), pharmaceuticals, pesticides, natural toxins, high production volume substances covered under the European REACH regulation (EC: 1272/2008), priority contaminants of emerging concern (CECs) and regulatory lists from NORMAN partners. Several lists focus on transformation products (TPs) and complex features detected in the environment with various levels of provenance and structural information. Each list is available for separate download. The merged, curated collection is also available as the NORMAN Substance Database (NORMAN SusDat). Both the NORMAN-SLE and NORMAN SusDat are integrated within the NORMAN Database System (NDS). The individual NORMAN-SLE lists receive digital object identifiers (DOIs) and traceable versioning via a Zenodo community (https://zenodo.org/communities/norman-sle), with a total of > 40,000 unique views, > 50,000 unique downloads and 40 citations (May 2022). NORMAN-SLE content is progressively integrated into large open chemical databases such as PubChem (https://pubchem.ncbi.nlm.nih.gov/) and the US EPA's CompTox Chemicals Dashboard (https://comptox.epa.gov/dashboard/), enabling further access to these lists, along with the additional functionality and calculated properties these resources offer. PubChem has also integrated significant annotation content from the NORMAN-SLE, including a classification browser (https://pubchem.ncbi.nlm.nih.gov/classification/#hid=101).

Conclusions
The NORMAN-SLE offers a specialized service for hosting suspect screening lists of relevance for the environmental community in an open, FAIR manner that allows integration with other major chemical resources. These efforts foster the exchange of information between scientists and regulators, supporting the paradigm shift to the "one substance, one assessment" approach. New submissions are welcome via the contacts provided on the NORMAN-SLE website (https://www.norman-network.com/nds/SLE/).

AbstractThe Partnership for Chemicals Risk Assessment (PARC) is currently under development as a joint research and innovation programme to strengthen the scientific basis for chemical risk assessment in the EU. The plan is to bring chemical risk assessors and managers together with scientists to accelerate method development and the production of necessary data and knowledge, and to facilitate the transition to next-generation evidence-based risk assessment, a non-toxic environment and the European Green Deal. The NORMAN Network is an independent, well-established and competent network of more than 80 organisations in the field of emerging substances and has enormous potential to contribute to the implementation of the PARC partnership. NORMAN stands ready to provide expert advice to PARC, drawing on its long experience in the development, harmonisation and testing of advanced tools in relation to chemicals of emerging concern and in support of a European Early Warning System to unravel the risks of contaminants of emerging concern (CECs) and close the gap between research and innovation and regulatory processes. In this commentary we highlight the tools developed by NORMAN that we consider most relevant to supporting the PARC initiative: (i) joint data space and cutting-edge research tools for risk assessment of contaminants of emerging concern; (ii) collaborative European framework to improve data quality and comparability; (iii) advanced data analysis tools for a European early warning system and (iv) support to national and European chemical risk assessment thanks to harnessing, combining and sharing evidence and expertise on CECs. By combining the extensive knowledge and experience of the NORMAN network with the financial and policy-related strengths of the PARC initiative, a large step towards the goal of a non-toxic environment can be taken.