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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

Abstract Increasing 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.

A collaborative trial involving 16 participants from nine European countries was conducted within the NORMAN network in efforts to harmonise suspect and non-target screening of environmental contaminants in whole fish samples of bream (Abramis brama). Participants were provided with freeze-dried, homogenised fish samples from a contaminated and a reference site, extracts (spiked and non-spiked) and reference sample preparation protocols for liquid chromatography (LC) and gas chromatography (GC) coupled to high resolution mass spectrometry (HRMS). Participants extracted fish samples using their in-house sample preparation method and/or the protocol provided. Participants correctly identified 9–69 % of spiked compounds using LC-HRMS and 20–60 % of spiked compounds using GC-HRMS. From the contaminated site, suspect screening with participants’ own suspect lists led to putative identification of on average ∼145 and ∼20 unique features per participant using LC-HRMS and GC-HRMS, respectively, while non-target screening identified on average ∼42 and ∼56 unique features per participant using LC-HRMS and GC-HRMS, respectively. Within the same sub-group of sample preparation method, only a few features were identified by at least two participants in suspect screening (16 features using LC-HRMS, 0 features using GC-HRMS) and non-target screening (0 features using LC-HRMS, 2 features using GC-HRMS). The compounds identified had log octanol/water partition coefficient (KOW) values from −9.9 to 16 and mass-to-charge ratios (m/z) of 68 to 761 (LC-HRMS and GC-HRMS). A significant linear trend was found between log KOW and m/z for the GC-HRMS data. Overall, these findings indicate that differences in screening results are mainly due to the data analysis workflows used by different participants. Further work is needed to harmonise the results obtained when applying suspect and non-target screening approaches to environmental biota samples.

Prenatal exposure to certain organic chemicals like pesticides and phenols has been lifelong associated with birth outcomes and health disorders. Many personal care product (PCP) ingredients have similar properties or structures to those chemicals. Previous studies have documented the occurrence of UV filters (UVFs) and paraben preservatives (PBs) in the placenta, but observational studies concerning PCPs chemicals and foetal exposure are particularly scarce. Thus, this work aimed to assess the presence of a wide range of PCPs chemicals using target and suspect screening in the umbilical cord blood of new born babies to evaluate their potential transfer to the fetus. To do so, we analysed 69 umbilical cord blood plasma samples from a mother–child cohort from Barcelona (Spain). We quantified 8 benzophenone-type UVFs and their metabolites, and 4 PBs using validated analytical methodologies based on target screening using liquid chromatography-tandem mass spectrometry (HPLC-MS/MS). Then, we screened for additional 3246 substances using high-resolution mass spectrometry (HRMS) and advanced suspect analysis strategies. Six UVFs and three parabens were detected in the plasma with frequencies between 1.4% and 17.4% and concentrations up to 53.3 ng/mL (benzophenone-2). Thirteen additional chemicals were tentatively identified in the suspect screening, and ten were further confirmed with the corresponding standards. Among them, we found the organic solvent N-methyl-2-pyrrolidone, the chelating agent 8-hydroxyquinoline, and the antioxidant 2,2′-methylenebis(4-methyl-6-tert-butylphenol), which have been demonstrated to display reproductive toxicity. UVFs and PBs presence in the umbilical cord blood demonstrates mother-fetus transfer through the placental barrier and prenatal exposure to these PCPs chemicals, which may lead to adverse effects in the early stages of fetal development. Considering the small cohort used in this study, the reported results should be interpreted as a preliminary reference for the background umbilical cord transfer levels of the target PCPs chemicals. Further research is needed to determine the long-term consequences of prenatal exposure to PCPs chemicals.

Little is known about the presence of organic pollutants in human brain (and even less in brain tumors). In this regard, it is necessary to develop new analytical protocols capable of identifying a wide range of exogenous chemicals in this type of samples (by combining target, suspect and non-target strategies). These methodologies should be robust and simple. This is particularly challenging for solid samples, as reliable extraction and clean-up techniques should be combined to obtain an optimal result. Hence, the present study focuses on the development of an analytical methodology that allows the screening of a wide range of organic chemicals in brain and brain tumor samples. This protocol was based on a solid-liquid extraction based on bead beating, solid-phase extraction clean-up with multi-layer mixed-mode cartridges, reconstitution and LCHRMS analysis. To evaluate the performance of the extraction methodology, a set of 66 chemicals (e.g., pharmaceuticals, biocides, or plasticizers, among others) with a wide range of physicochemical properties was employed. Quality control parameters (i.e., linear range, sensitivity, matrix effect (ME%), and recoveries (R%)) were calculated and satisfactory results were obtained for them (e.g., R% within 60–120% for 32 chemicals, or ME% higher than 50% (signal suppression) for 79% of the chemicals).

Measurement(s) chemical • drinking water Technology Type(s) high resolution mass spectrometry • non-target analysis • Interlaboratory Factor Type(s) method Sample Characteristic - Environment laboratory environment Machine-accessible metadata file describing the reported data: https://doi.org/10.6084/m9.figshare.15028665

The Spanish Mediterranean basin is particularly susceptible to climate change and human activities, making it vulnerable to the influence of anthropogenic contaminants. Therefore, conducting comprehensive and exhaustive water quality assessment in relevant water bodies of this basin is pivotal. In this work, surface water samples from coastal lagoons or estuaries were collected across the Spanish Mediterranean coastline and subjected to target and suspect screening of 1,585 organic micropollutants by liquid chromatography coupled to ion mobility separation and high resolution mass spectrometry. In total, 91 organic micropollutants could be confirmed and 5 were tentatively identified, with pharmaceuticals and pesticides being the most prevalent groups of chemicals. Chemical analysis data was compared with data on bioanalysis of those samples (recurrent aryl hydrocarbon receptor (AhR) activation, and estrogenic receptor (ER) inhibition in wetland samples affected by wastewater streams). The number of identified organic contaminants containing aromatic rings could explain the AhR activation observed. For the ER antagonistic effects, predictions on estrogenic inhibition potency for the detected compounds were used to explain the activities observed. The integration of chemical analysis with bioanalytical observations allowed a comprehensive overview of the quality of the water bodies under study.

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 (

This work describes a robust and powerful method for wide-scope target and non-target analysis of xenobiotics in biota samples based on bead beating tissuelyser extraction, solid phase extraction (SPE) clean-up and further detection by liquid chromatography coupled to high resolution mass spectrometry (LC-HRMS). Unlike target methodologies, non-target methods usually aim at determining a wide range of still unknown substances with different physicochemical properties. Therefore, losses during the extraction process were minimised. Apart from that, the reduction of possible interferences showed to be necessary to expand the number of compounds that can be detected. This was achieved with an additional SPE clean-up step carried out with mixed-bed multi-layered cartridges. The method was validated with a set of 27 compounds covering a wide range of physicochemical properties, and further applied to the analysis of krill and fish samples. • The bead beating extraction was efficient for a wide range of organic pollutants in small quantities of biota samples. • Multi-layered solid phase extraction clean-up yield a wide xenobiotics coverage reducing matrix effects. • Method validation with 27 compounds led to a suitable method for non-target analysis of organic pollutants in biota.

UV filters and parabens are compounds used in large quantities in modern societies and have become ubiquitous in the environment. They are considered compounds of emerging concern due to the unwanted effects they cause in the environment and their bioaccumulation potential in humans. Considering their endocrine disrupting activity and their so far unknown effects in newborns, a continuous monitoring of these substances is required. In this work, we developed and validated a new sensitive methodology for the analysis of 8 UV filters and metabolites, and 4 parabens in umbilical cord blood samples. The method consisted of a liquid-liquid extraction and phase separation by freezing. Then, the organic extract was further analyzed at alkaline pH using liquid chromatography coupled to tandem-mass spectrometry (LC-MS/MS) using a QqLIT hybrid mass spectrometer as analyzer. The low limits of detection achieved (0.01–0.42 ng/mL) allowed the reliable simultaneous quantification of UV filters and parabens in this complex biological matrix. • Simple, fast and sensitive analysis of UV filters and parabens in cord blood samples. • First simultaneous analysis of UV filters and parabens in cord blood. • Allows the evaluation of perinatal transfer of UV filters and parabens from the mother to the fetus.

Vinasse, a liquid waste which originates from the production of ethanol fuel from sugarcane, has been widely used as soil amendment in Brazil. An important concern that arises from vinasse reuse is the dissemination of antibiotics to the environment through crop soils. This work evaluated the performance of Pressurized Liquid Extraction (PLE) and QuEChERS (quick, easy, cheap, effective, rugged and safe) to extract several multiple-class antibiotics, such as cephalosporins, fluoroquinolones, ionophores, lincosamides, macrolides, quinolones, streptogramin, sulfonamides, tetracyclines and others, from agricultural soils. The performance of several parameters was evaluated for both PLE and QuEChERS, such as the extraction temperature (for PLE), solvents composition, pH and the addition of EDTA. Both methods were able to extract most target antibiotics. However, QuEChERS showed higher recoveries for macrolides and nitroimidazoles, while PLE was more suitable for fluoroquinolones and ionophores (i.e. monensin). The use of citrate-phosphate buffer at pH 7.0, in combination with methanol for PLE and with acetonitrile for QuEChERS, provided the highest antibiotic recoveries for both methods. The use of EDTA did not increase antibiotic recovery rates for QuEChERS, while the temperature had almost no influence on the extraction efficiency in PLE. • Citrate-phosphate buffer at pH 7.0 provided higher antibiotic recoveries for QuEChERS and PLE. • The combination buffer-methanol provided higher recoveries for PLE. • QuEChERS and PLE methods were able to extract most of the target antibiotics.