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A time-trend guided non-target screening study of organic contaminants in Baltic Sea harbor porpoise (1988–2019), guillemot (1986–2019), and white-tailed sea eagle (1965–2017) using gas chromatography–high-resolution mass spectrometry
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)
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. 829, article id 154620Article in journal (Refereed) Published
Abstract [en]

The rate of decline in regulated persistent organic pollutant (POP) concentrations in Baltic Sea biota has leveled off in recent years, with new contaminants frequently being discovered. There is, therefore, a need for comprehensive approaches to study occurrence and temporal trends of a wide range of environmental contaminants, including legacy POPs, contaminants of emerging concern (CECs), and new contaminants. In the current work, non-target screening (NTS) workflows were developed and used for, to the best of our knowledge, the first time-trend directed NTS of biota using gas chromatography–high-resolution mass spectrometry (GC-HRMS). To maximize contaminant coverage, both electron ionization (EI) and electron capture negative ion chemical ionization (ECNI) were used. The EI data were treated using highly automated workflows to find, prioritize, and tentatively identify contaminants with statistically significant temporal trends. The ECNI data were manually processed and reviewed prior to time-trend analysis. Altogether, more than 300 tentatively identified contaminants were found to have significant temporal trends in samples of Baltic guillemot, harbor porpoise, or white-tailed sea eagle. Significant decreases were found for many regulated chemicals, as could be expected, such as PCBs, polychlorinated terphenyls, chlorobenzenes, toxaphenes, DDT, other organochlorine pesticides, and tri- and tetra- bromodiphenyl ethers (BDEs). The rate of decline of legacy POPs agreed well with data reported from targeted analyses. Significant increases were observed for small polycyclic aromatic hydrocarbons, heptaBDEs, CECs, and terpenes and related compounds. The CECs included, among others, one plasticizer tributyl acetylcitrate (ATBC), two antioxidants 2,6-bis(1,1-dimethylethyl)phenol and 2,6-bis(tert-butyl)-4-(4-morpholinyl-methyl)phenol, and two compounds used in polymer production, trimethyl isocyanurate and 2-mercaptobenzothiazole, which had not previously been reported in biota. Their increased concentrations in biota indicate increased use and release. The increase in ATBC may be linked to increased use of it as a substitute for di-2-ethylhexyl phthalate (DEHP), which has been phased out over the last decade.

Place, publisher, year, edition, pages
Elsevier, 2022. Vol. 829, article id 154620
Keywords [en]
Temporal trends, Non-target screening, GC-HRMS, Contaminants of emerging concern, The Baltic Sea, Top consumer species
National Category
Environmental Sciences
Research subject
environmental science
Identifiers
URN: urn:nbn:se:umu:diva-193243DOI: 10.1016/j.scitotenv.2022.154620ISI: 000793203100012PubMedID: 35306077Scopus ID: 2-s2.0-85126536226OAI: oai:DiVA.org:umu-193243DiVA, id: diva2:1646354
Funder
Mistra - The Swedish Foundation for Strategic Environmental ResearchAvailable from: 2022-03-22 Created: 2022-03-22 Last updated: 2024-07-02Bibliographically 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, AndriyGallampois, ChristineHaglund, Peter

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