Identification of Mutagenic Aromatic Amines in River Samples with Industrial Wastewater Impact

Muz, Melis; Dann, Janek Paul; Jäger, Felix; Brack, Werner; Krauß, Martin

doi:10.1021/acs.est.7b00426

Cited by 42 publications

(45 citation statements)

References 47 publications

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“…Sample preparation and analytical settings of LC-HRMS are given in the Supplemental Data, Section S4). Nontarget screening (NTS) of the PR-active secondary fraction F18.4 was carried out as described previously (Muz et al 2017a). Briefly, samples (F18.4 and blanks) were initially screened…”

Section: Chemical Analysismentioning

confidence: 99%

Effect‐Directed Analysis of Progestogens and Glucocorticoids at Trace Concentrations in River Water

Hashmi

Krauß

Escher

et al. 2019

Enviro Toxic and Chemistry

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Effect-based monitoring is increasingly applied to detect and-in conjunction with chemical analysis-to identify endocrine-disrupting compounds (EDCs) in the environment. Although this approach of effect-directed analysis has been successfully demonstrated for estrogenicity and androgenicity, data on progestogens and glucocorticoids driving endocrine disruption are quite limited. We investigated progestogenic and glucocorticoid activities in Danube River water receiving untreated wastewater from Novi Sad, Serbia. After a 2-step fractionation, all fractions were tested with reporter gene bioassays for agonistic and antagonistic hormonal responses at progestogenic and glucocorticoid hormone receptors as well as with target and nontarget analytical screening of active fractions by liquid chromatography-high-resolution mass spectrometry. Due to masking by cytotoxic mixture components, the effects could not be detected in the raw water extract but were unraveled only after fractionation. Target chemical screening of the fraction that was active in the progesterone receptor (PR) assay revealed that progesterone and megestrol acetate were predominant drivers of PR-mediated activity along with medroxyprogesterone, dihydrotestosterone, androsterone, and epiandrosterone. Hydrocortisone was detected at sub-ng/L concentration in the active fraction in the glucocorticoid receptor (GR) assay but could not explain a significant fraction of the observed GR activity. The present study indicates that effect-based monitoring is a powerful tool to detect EDCs in the aquatic environment but that fractionation may be required to avoid masking effects of mixture components. Future effect-directed analysis studies are required to better understand the occurrence of EDCs and masking compounds in different lipophilicity windows, to finally reduce fractionation requirements for monitoring to a smart clean-up. Environ

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Section: Chemical Analysismentioning

confidence: 99%

Effect‐Directed Analysis of Progestogens and Glucocorticoids at Trace Concentrations in River Water

Hashmi

Krauß

Escher

et al. 2019

Enviro Toxic and Chemistry

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“…These inputs might contain highly specific substances or substances in much higher concentrations as compared to municipal wastewater (e.g. [14,41,43]).…”

Section: Introductionmentioning

confidence: 99%

Prioritising site-specific micropollutants in surface water from LC-HRMS non-target screening data using a rarity score

et al. 2019

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Background: Current compound prioritisation and monitoring approaches within Europe focus mainly on widely occurring priority and river basin specific pollutants but may overlook site-specific contamination from local emission sources. Thus, we propose a robust and semiautomated approach for the identification of site-specific chemicals and a prioritisation of water bodies with specific contamination based on non-target screening data from liquid chromatography coupled to high-resolution mass spectrometry. Results: For prioritisation of site-specific contaminants, we calculated rarity scores for all peaks occurring in a set of 31 surface water samples, which combine the maximum signal intensity of a peak in a dataset with its frequency of occurrence in that dataset in one single number. These were a robust measure without the need to address the problems of missing data in more sophisticated multivariate statistical methods. For our dataset, site-specific compounds were defined for rarity scores > 1000, and the studied 31 sites showed a huge difference in the number of such peaks (0-91 in positive and 0-48 in negative ion mode). Together with isotopologue detection, the evaluation of mass defects and the occurrence of homologue series, which all could be obtained from automated data processing, a more detailed characterisation of these site-specific contaminations was possible. For three selected sites with a high number of site-specific peaks, novel or unexpected compounds could be identified, which stem from specific usage or (former) industrial production upstream of these sites. Conclusions and outlook: The proposed approach allows for a rapid screening of large non-target screening datasets for site-specific contaminants, the prioritisation of sites with such a specific contamination and the subsequent identification of these compounds. Thus, the risk of overlooking possibly hazardous chemicals (including unknowns) which are not covered in conventional monitoring and prioritisation schemes is reduced.

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“…After specific derivatization techniques were applied [44], several of these compounds could be identified. The intensity of two peaks, in fact two diaminophenazine isomers, were found to correlate with mutagenicity and were eventually confirmed as the drivers of the observed mutagenicity [45].…”

Section: Sufficient Variance (Larger Than the Data Uncertainty)mentioning

confidence: 75%

Future water quality monitoring: improving the balance between exposure and toxicity assessments of real-world pollutant mixtures

et al. 2019

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Environmental water quality monitoring aims to provide the data required for safeguarding the environment against adverse biological effects from multiple chemical contamination arising from anthropogenic diffuse emissions and point sources. Here, we integrate the experience of the international EU-funded project SOLUTIONS to shift the focus of water monitoring from a few legacy chemicals to complex chemical mixtures, and to identify relevant drivers of toxic effects. Monitoring serves a range of purposes, from control of chemical and ecological status compliance to safeguarding specific water uses, such as drinking water abstraction. Various water sampling techniques, chemical target, suspect and non-target analyses as well as an array of in vitro, in vivo and in situ bioanalytical methods were advanced to improve monitoring of water contamination. Major improvements for broader applicability include tailored sampling techniques, screening and identification techniques for a broader and more diverse set of chemicals, higher detection sensitivity, standardized protocols for chemical, toxicological, and ecological assessments combined with systematic evidence evaluation techniques. No single method or combination of methods is able to meet all divergent monitoring purposes. Current monitoring approaches tend to emphasize either targeted exposure or effect detection. Here, we argue that, irrespective of the specific purpose, assessment of monitoring results would benefit substantially from obtaining and linking information on the occurrence of both chemicals and potentially adverse biological effects. In this paper, we specify the information required to: (1) identify relevant contaminants, (2) assess the impact of contamination in aquatic ecosystems, or (3) quantify cause-effect relationships between contaminants and adverse effects. Specific strategies to link chemical and bioanalytical information are outlined for each of these distinct goals. These strategies have been developed and explored using case studies in the Danube and Rhine river basins as well as for rivers of the Iberian Peninsula. Current water quality assessment suffers from biases resulting from differences in approaches and associated uncertainty analyses. While exposure approaches tend to ignore data gaps (i.e., missing contaminants), effect-based approaches penalize data gaps with increased uncertainty factors. This integrated work suggests systematic ways to deal with mixture exposures and combined effects in a more balanced way, and thus provides guidance for future tailored environmental monitoring. which permits unrestricted use, distribution, and reproduction in any medium, provided you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made.

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Identification of Mutagenic Aromatic Amines in River Samples with Industrial Wastewater Impact

Cited by 42 publications

References 47 publications

Effect‐Directed Analysis of Progestogens and Glucocorticoids at Trace Concentrations in River Water

Effect‐Directed Analysis of Progestogens and Glucocorticoids at Trace Concentrations in River Water

Prioritising site-specific micropollutants in surface water from LC-HRMS non-target screening data using a rarity score

Future water quality monitoring: improving the balance between exposure and toxicity assessments of real-world pollutant mixtures

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