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Comprehensive non-target screening of biomagnifying organic contaminants in the Baltic Sea food web
Umeå University, Faculty of Science and Technology, Department of Chemistry. (EcoChange)ORCID iD: 0000-0002-0090-809X
Umeå University, Faculty of Science and Technology, Department of Chemistry. (EcoChange)ORCID iD: 0000-0003-2293-7913
2022 (English)In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 851, article id 158280Article in journal (Refereed) Published
Abstract [en]

High-resolution mass spectrometry (HRMS) based non-target screening (NTS) is a powerful approach for the simultaneous determination of multiple environmental contaminant classes in complex biota samples. In this study, trophic biomagnification factor (TMF) directed NTS was performed to find and (tentatively) identify known, emerging, and new chemical contaminants that are persistent and biomagnify in Baltic Sea biota. The investigated food web included seven species: one filter feeder (blue mussel, Mytilus edulis), two fish (eelpout, Zoarces viviparous; herring, Clupea harengus), two marine mammals (harbor porpoise, Phocoena phocoena; grey seal, Halichoerus grypus) and two birds (guillemot, Uria aalge; white-tailed sea eagle, Haliaeetus albicilla). The NTS procedure included extraction with organic solvent mixtures, two-step high-resolution gel permeation chromatography clean-up, Florisil® fractionation, gas chromatography (GC) HRMS analysis in electron ionization (EI) and electron capture negative ion chemical ionization (ECNI) modes, and NTS data processing. The latter was performed differently for the EI and ECNI data: the EI data were treated using a flexible and highly automated TMF-directed NTS workflow, whereas the ECNI data were treated with a simpler and less automated workflow that specifically screened for brominated compounds. The two workflows collectively revealed biomagnification (statistically significant TMF values) of >250 tentatively identified compounds, including legacy persistent organic pollutants (POPs), such as PCBs and PCB-related compounds, DDT and its metabolites, and organochlorine pesticides (OCPs), contaminants of emerging concern (CECs), and halogenated natural products (HNPs). Among the tentatively identified CECs, nine have not previously been reported in environmental biota samples. These included four polymer additives (used as antioxidants, rubber additives or plasticizers) and two cosmetic product additives (ethyl myristate and isopropyl palmitate). The CECs should be prioritized for future structure verification and quantification using reference standards.

Place, publisher, year, edition, pages
Elsevier, 2022. Vol. 851, article id 158280
Keywords [en]
Non-target screening, Biomagnification, Trophic magnification factors, GC-HRMS, Contaminants of emerging concern, Baltic Sea
National Category
Environmental Sciences
Research subject
environmental science
Identifiers
URN: urn:nbn:se:umu:diva-198941DOI: 10.1016/j.scitotenv.2022.158280ISI: 000874763100008PubMedID: 36029819Scopus ID: 2-s2.0-85136591772OAI: oai:DiVA.org:umu-198941DiVA, id: diva2:1690964
Funder
Mistra - The Swedish Foundation for Strategic Environmental ResearchBONUS - Science for a better future of the Baltic Sea region, Art. 185Available from: 2022-08-29 Created: 2022-08-29 Last updated: 2023-09-05Bibliographically approved
In thesis
1. Comprehensive non-target screening to find and identify new biomagnifying organic contaminants in Baltic Sea top consumers
Open this publication in new window or tab >>Comprehensive non-target screening to find and identify new biomagnifying organic contaminants in Baltic Sea top consumers
2022 (English)Doctoral thesis, comprehensive summary (Other academic)
Alternative title[sv]
Bred screening för att finna och identifiera nya biomagnifierande organiska föroreningar i toppkonsumenter i Östersjön
Abstract [en]

The development of industrial processes in the 19th and 20th centuries, in particular oil refining, resulted in a huge discovery and subsequent large-scale production of a variety of chemicals. These useful chemicals supposedly made the everyday lives of people easier and better by, for instance, controlling the spread of diseases such as malaria, through the use of DDT and other organochlorine pesticides (OCPs).

During the 1970s and following decades, it was hypothesized and later shown, that these, and other “helpful chemicals” such as polychlorinated biphenyls (PCBs), played a crucial role in the steep population decline observed for multiple species in the Baltic Sea. They were classified as anthropogenic (man-made) hazardous substances (AHSs). Many AHSs can be stored in fatty tissues of the organisms and magnify in species at high trophic levels (predators) of the food web, as a result of persistence and transfer from lower-level organisms (prey). This process is called biomagnification and is characterized by biomagnification or trophic magnification factors (BMFs or TMFs, respectively). AHSs can be roughly divided into known chemicals of concern, such as persistent organic pollutants (POPs), and contaminants of emerging concern (CECs), that include novel flame retardants, polymer additives, and many more. Both the production and use of a number of AHSs have been regulated since the 1970s. To understand the outcome of the regulations, retrospective analysis of samples from different years, a time-trend study, is often utilized.

The main aim of this work was to develop a non-selective sample extraction, purification, and analysis method, and then find and identify as many biomagnifying contaminants as possible. To assess both biomagnification and temporal trends of a wide range of chemical contaminants in a given Baltic Sea food web, non-target screening (NTS) was used. A clean-up method was established and tested with a satisfactory outcome: processed extracts were pure enough for gas chromatography-mass spectrometry (GC-MS) analysis. Also, accompanying NTS data processing workflows were developed. Application of these resulted in BMFs for more than 100 contaminants (Paper I). The data processing workflow was refined for faster detection of chemicals that demonstrate temporal trends and/or biomagnify. It was possible to detect and tentatively identify more than 300 legacy POPs and CECs with statistically significant temporal trends in three Baltic top consumers (Paper II). Adjusted NTS workflows were used to reveal more than 250 compounds that possessed trophic magnification properties (Paper III). Inspired by the discovery of a novel flame retardant Dechlorane 602 (Paper I), a suspect screening for dechlorane-related compounds and their transformation products was carried out. A total of 31 compounds were detected and tentatively identified, many of which showed significant temporal trends and biomagnification (Paper IV). A number of compounds reported in Papers I–IV were tentatively identified for the first time in wildlife. In addition, the papers provide valuable spectral and retention information for the researchers in the field.

In conclusion, this thesis presents useful GC-MS-based NTS workflows and biomagnification or time-trend data for a plethora of organic contaminants in the Baltic Sea food web. The data can contribute to i) the assessment of the influence pollutants have on the ecosystem and ii) various mitigation actions for AHSs, such as evaluating dechloranes for regulation under the Stockholm Convention on POPs, helping in the fight for a better environment and future.

Place, publisher, year, edition, pages
Umeå: Umeå University, 2022. p. 69
Keywords
Baltic Sea, persistent organic pollutants, contaminants of emerging concern, non-target screening, GC-MS, biomagnification, temporal trends
National Category
Analytical Chemistry
Research subject
Analytical Chemistry; environmental science
Identifiers
urn:nbn:se:umu:diva-199058 (URN)978-91-7855-833-9 (ISBN)978-91-7855-834-6 (ISBN)
Public defence
2022-09-30, Lilla hörsalen, KBE301, KBC-huset, Umeå, 10:00 (English)
Opponent
Supervisors
Available from: 2022-09-09 Created: 2022-09-02 Last updated: 2024-07-02Bibliographically approved

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Rebryk, AndriyHaglund, Peter

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