Abstract
Abstract
Background
Sediments are sinks for organic micropollutants, which are traditionally analysed by gas chromatography–mass spectrometry (GC–MS). Although GC–MS and GC–tandem MS (MS/MS) are preferred for target screening, they provide only limited chromatographic resolution for nontarget screening. In this study, a comprehensive two-dimensional GC–high-resolution MS method (GC × GC–HRMS) was developed for nontarget screening and source identification of organic micropollutants in sediments from an urban channel and adjacent lake in Copenhagen, Denmark. The GC × GC–HRMS data were processed by pixel-based chemometric analysis using baseline subtraction, alignment, normalisation, and scaling before principal component analysis (PCA) of the pre-processed GC × GC–HRMS base peak ion chromatograms (BPCs). The analysis was performed to identify organic micropollutants of high abundance and relevance in the urban sediments and to identify pollution sources. Tentative identifications were based on match factors and retention indices and tagged according to the level of identification confidence.
Results
The channel contained both a significantly higher abundance of micropollutants and a higher diversity of compounds compared to the lake. The PCA models were able to isolate distinct sources of chemicals such as a natural input (viz., a high relative abundance of mono-, di- and sesquiterpenes) and a weathered oil fingerprint (viz., alkanes, naphthenes and alkylated polycyclic aromatic hydrocarbons). A dilution effect of the weathered oil fingerprint was observed in lake samples that were close to the channel. Several benzothiazole-like structures were identified in lake samples close to a high-traffic road which could indicate a significant input from asphalt or tire wear particles. In total, 104 compounds and compound groups were identified.
Conclusions
Several chemical fingerprints of different sources were described in urban freshwater sediments in Copenhagen using a pixel-based chemometric approach of GC × GC–HRMS BPCs. Various micropollutants of anthropogenic origin were identified. Tailored pre-processing and careful interpretation of the identification results is inevitable and still requires further research for an automated workflow.
Publisher
Springer Science and Business Media LLC
Reference35 articles.
1. Connor R, Uhlenbrook S, Koncagül E, Ortigara ARC (2017) The United Nations world water development report 2017—wastewater, an untapped resource; executive summary. WWAP: United Nations
2. Schwarzenbach RP, Escher BI, Fenner K, Hofstetter TB, Johnson CA, von Gunten U, Wehrli B (2006) The challenge of micropollutants in aquatic systems. Science 313:1072–1077. https://doi.org/10.1126/science.1127291
3. Veenaas C, Bignert A, Liljelind P, Haglund P (2018) Nontarget screening and time-trend analysis of sewage sludge contaminants via two-dimensional gas chromatography-high resolution mass spectrometry. Environ Sci Technol 52:7813–7822. https://doi.org/10.1021/acs.est.8b01126
4. European Parliament and Council (2013) Directive 2013/39/EU of the European Parliament and of the Council of 12 August 2013 amending Directives 2000/60/EC and 2008/105/EC as regards priority substances in the field of water policy Text with EEA relevance. Official Journal of the European Union L226/1
5. Reiner EJ, Jobst KJ, Megson D, Dorman FL, Focant J-F (2014) Analytical methodology of POPs. In: O’Sullivan G, Sandau C (eds) Environmental forensics for persistent organic pollutants. Elsevier, Amsterdam
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