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Temporal trends from 1981 to 2013 of 28 per‐ and polyfluoroalkyl substances (PFASs) were investigated in liver tissue of cod (Gadus morhua) sampled near southeast Gotland, in the Baltic Sea. A total of 10 PFASs were detected, with ∑28PFAS geometric mean concentrations ranging from 6.03 to 23.9 ng/g ww. Perfluorooctane sulfonate (PFOS) was the predominant PFAS, which increased at a rate of 3.4% per year. Most long‐chain perfluoroalkyl carboxylic acids increased at rates of 3.9 to 7.3% per year except for perfluorooctanoate (PFOA), which did not change significantly over time. The perfluoroalkyl acid precursors perfluorooctane sulfonamide (FOSA) and 6:2 fluorotelomer sulfonic acid were detected, of which the former (FOSA) declined at a rate of –4.4% per year, possibly reflecting its phase‐out starting in 2000. An alternate time trend analysis from 2000 to 2013 produced slightly different results, with most compounds increasing at slower rates compared to the entire study period. An exception was perfluorohexane sulfonate (PFHxS), increasing at a faster rate of 3.7% measured from 2000 on, compared to the 3.0% per year measured starting from 1981. Analysis of the total fluorine content of the samples revealed large amounts of unidentified fluorine; however, its composition (organic or inorganic) remains unclear. Significant negative correlations were found between concentrations of individual PFASs (with the exception of PFOS) and liver somatic index. In addition, body length was negatively correlated with PFOA and perfluorononanoate, but positively correlated with perfluorododecanoate (PFDoDA) and FOSA. Additional studies on endocrine, immunological, and metabolic effects of PFAS in marine fish are essential to assess the environmental risk of these substances. Environ Toxicol Chem 2020;39:300–309. © 2019 SETAC, Increasing trends for most long‐chain perfluoroalkyl acids and declining FOSA concentrations were detected in Baltic cod liver, along with correlations of certain PFASs with body length and liver somatic index.

Per- and poly-fluoroalkyl substances (PFAS) are a problematic group of chemicals used in various industrial and household products. They have been extensively detected in wastewater as a result of day-to-day product usage. Due to concerns about their safety, voluntary and regulatory action to limit the manufacture and use of some individual PFAS has occurred since the year 2000. The impact that this intervention has had on the use and potential exposure of Australians has not been measured. Wastewater serves as a powerful tool to assess the chemical use or consumption patterns of a population over time. We accessed a ten-year wastewater archiving program to conduct a temporal analysis of PFAS trends in an urban Australian population between the years 2010 and 2020. Results showed a decline in the concentrations for most PFAS, and a change in the PFAS profile from perfluorosulfonic acids and long-chain perfluorocarboxylic acids, to the short-chain perfluorocarboxylic acids and PFOS-replacement degradation products such as 5:3 FTCA. Intermittent pulses of PFAS that were significantly higher than ‘background’ levels (i.e., representing the PFAS input from primarily households) were observed, suggesting continuing industrial PFAS input within the wastewater catchment. This study highlights the long-term consequences of the diffuse use of persistent chemicals in products, and their ability to continue to enter the wastewater stream for decades.

Hydroxylated polybrominated diphenyl ethers (OH-PBDEs), naturally produced by algae and cyanobacteria in the Baltic Sea, are potent disrupters of energy metabolism as well as endocrine disruptors and neurotoxins. In this study, European perch (Perca fluviatilis) from the Baltic Sea were sampled from May until October. OH-PBDEs and ten biomarkers were measured in each individual (n = 84 over 18 sampling time points) to study potential correlations between exposure to OH-PBDEs and changes in biomarkers. Several biomarkers showed significant non-linear seasonal variation. In the perch, ethoxyresorufin-O-deethylase (EROD) activity, plasma lactate concentration, and plasma glucose concentration showed a significant positive log-linear correlation with OH-PBDEs, whereas lipid percentage and liver somatic index showed a significant negative log-linear correlation with OH-PBDEs. These results strengthen the concern that OH-PBDEs could cause negative health effects for fish in the Baltic Sea.

Organochlorine (OCPs) and organophosphorus pesticides (OPPs) have been intensively applied in rice paddy field farming to control pest infestation and increase the yield. In this study, we investigated the presence of organochlorine and organophosphorus pesticides in paddy rice and soil from rice plantations in Thailand and China. According to concentration and distribution of OCPs, the most abundant OCPs residues in rice and soil from Thailand and China were dichlorodiphenyltrichloroethane and hexachlorocyclohexanes. The OPPs of methidathion, carbophenothion, chlorpyrifos, and diazinon were common to Thailand and China in both types of samples. The detection frequency of multiple types of these pesticides was greater than 50% of total samples. The relative concentration of some OPPs residues in rice and soil from Thailand and China were significantly different from each other (p &lt, 0.0083), whereas, no significant difference was observed for the relative concentration of OCPs residues in rice and soil from both countries, except for HCHs (p &lt, 0.05). Bioaccumulation factors of OCPs between rice and soil samples indicated that OCPs and OPPs in soil could accumulate in rice. The carcinogenic and non- carcinogenic risks of OCPs and OPPs seem to be in the safe range as recommended by the European Union.

Limited information exists regarding contemporary and historical emissions for many anthropogenic chemicals, especially for contaminants of emerging concern (CECs). This study examined temporal trends of several perfluoroalkyl substances (PFASs), polybrominated diphenyl ethers (PBDEs), and hexabromocyclododecanes (HBCDs) in three beluga whale (Delphinapterus leucas) populations from the Canadian Arctic [Hendrickson Island (HI), NT; Pangnirtung (PG), NU; and Sanikiluaq (SQ), NU] collected from 1982 to 2013. The confounding factors of animal size, age, and sex were included in the analyses, but were only significant for some CECs. The strongest temporal resolution was obtained from HI, which showed increasing trends in PBDEs (4.8%/year) and HBCDs (2.9%/year), and decreases in perfluoroalkylcarboxylic acids (PFCAs, −6.0%/year). Concentrations of perfluorooctanesulfonate (PFOS) were relatively stable between 1984 and 2010, increasing substantially in 2011; trends in perfluorooctanesulfonamide (PFOSA) concentrations were not strictly linear over the study period. PBDE, HBCD, and PFCA trends in the HI population were opposite/different to that of many other arctic animals (e.g., polar bears) for the same time period. Trends were inconsistent among locations, suggesting that regional differences in dietary exposure and/or sources may also impact these trends. The effects of climate-change-driven processes on the exposure and distribution of CECs are currently not well understood, highlighting a need for ongoing contaminant monitoring.

Nondestructive sample cleanup and comprehensive two-dimensional gas chromatography (GC×GC) high-resolution mass spectrometry (HRMS) analysis generated a massive amount of data that could be used for nontarget screening purposes. We present a data reduction and prioritization strategy that involves time-trend analysis of nontarget data. Sewage sludge collected between 2005 and 2015 in Stockholm (Sweden) was retrieved from an environmental specimen bank, extracted, and analyzed by GC×GC-HRMS. After data alignment features with high blank levels, artifacts and low detection frequency were removed. Features that appeared in four to six out of ten years were reprocessed to fill in gaps. The total number of compounds was reduced by more than 97% from almost 60 000 to almost 1500. The remaining compounds were analyzed for monotonic (log-linear) and nonmonotonic (smoother) time trends. In total, 192 compounds with log-linear trends and 120 compounds with nonmonotonic trends were obtained, respectively. Most compounds described by a log-linear trend exhibited decreasing trends and were traffic-related. Compounds with increasing trends included UV-filters, alkyl-phenols, and flavor and fragrances, which often could be linked to trade statistics. We have shown that nontarget screening and stepwise reduction of data provides a simple way of revealing significant changes in emissions of chemicals in society.

Short-, medium-, and long-chain chlorinated paraffins (SCCPs, MCCPs, and LCCPs) were analyzed in human milk from the Yangtze River Delta (YRD) and Scandinavia. Individual samples were collected from Shanghai, Jiaxing, and Shaoxing (China), Stockholm (Sweden), and Bodø (Norway) between 2010 and 2016. Mean concentrations (range) of SCCPs, MCCPs, and LCCPs in samples from the YRD were 124 [

A combined method for quantitative, suspect, and non-target screening of per- and polyfluoroalkyl substances (PFASs) was developed using ultra-high pressure liquid chromatography-ultra-high resolution (Orbitrap) mass spectrometry. The method was applied together with measurements of total- and extractable organofluorine (TF and EOF, respectively), to pooled serum samples from 1996–2017 from first-time mothers living in the county of Uppsala, Sweden, some of which were exposed to drinking water contaminated with perfluorohexane sulfonate (PFHxS) and other PFASs until mid-2012. Declining trends were observed for all target PFASs as well as TF, with homologue-dependent differences in year of onset of decline. Only 33% of samples displayed detectable EOF, and amongst these samples the percentage of EOF explained by target PFASs declined significantly (−3.5% per year) over the entire study period. This finding corroborates prior observations in Germany after the year 2000, and may reflect increasing exposure to novel PFASs which have not yet been identified. Non-target time trend screening revealed 3 unidentified features with time trends matching PFHxS (Spearman’s ρ > 0.5). These features require further investigation, but may represent contaminants which co-occurred with PFHxS in the contaminated drinking water.

Within the Swedish National Monitoring Programme for Contaminants in Freshwater Biota, perch, pike and Arctic char are being analysed from 32 lakes distributed all over Sweden. One of the main objectives of the monitoring has been to detect temporal trends in different areas and for different contaminants. However, the measured concentrations in biota can be affected by biological factors such as age, length, trophic position (TP), fat or dry weight content. A change in one or several of these variables over time, or even among specimens taken within the same year, is likely to result in an increased variation of the measured concentrations and hence in a lower chance of detecting a trend. The purpose of this study was to evaluate if an adjustment of contaminant time trends by primarily stable isotopes, but also other confounding factors can: A) reduce the individual and between-year variation and hence B) improve the likelihood of detecting temporal trends in time series for metals and organic contaminants. The study revealed an improvement in the likelihood of detecting a contaminant trend after adjustment of the data for almost all lakes and for all tested substances. For some lakes and substances, this improvement was substantial. Age seems to be an important confounding factor for metals and per- and polyfluoroalkyl substances. For lipophilic substances, fat content also appears to be an important factor in some lakes together with adjustments for carbon and nitrogen isotope ratios (d13C and d15N), which all reduced the variation in contaminant data. This suggests that there is a benefit of adjusting data on a regular basis in contaminant monitoring programmes in the future.

Additional file 3. Articles not used.

Additional file 8. Reported time trends or changes in concentrations.

Additional file 1. List of abbreviations.

Additional file 4. Critical appraisal checklist.

A combined method for quantitative analysis, along with suspect and non-target screening of per- and polyfluoroalkyl substances (PFAS) was developed using ultra-high pressure liquid chromatography-ultra-high resolution (Orbitrap) mass spectrometry. The method was applied together with measurements of total- and extractable organofluorine (TF and EOF, respectively), to pooled serum samples from 1996–2017 from first-time mothers living in the county of Uppsala, Sweden, some of which (i.e. 148 of 472 women sampled 1996–2012) were exposed to drinking water contaminated with perfluorohexane sulfonate (PFHxS) and other PFAS until mid-2012. Declining trends were observed for all target PFAS as well as TF, with homologue-dependent differences in year of onset of decline. Only 33% of samples displayed detectable EOF, and amongst these samples the percentage of EOF explained by target PFAS declined significantly (−3.5% per year) over the entire study period. This finding corroborates prior observations in Germany after the year 2000, and may reflect increasing exposure to novel PFAS which have not yet been identified. Suspect screening revealed the presence of perfluoro-4-ethylcyclohexanesulfonate (PFECHS), which displayed declining trends since the year 2000. Non-target time trend screening revealed 3 unidentified features with time trends matching PFHxS. These features require further investigation, but may represent contaminants which co-occurred with PFHxS in the contaminated drinking water.

Additional file 7. Reanalysed time trends.

Additional file 2. Searches.

The report deals with temporal trends of measured concentrations of representative congeners of dioxin-like PCBs, dioxins (PCDDs) and furans (PCDFs) (here together called dioxins) in biological samples from the Swedish marine and freshwater environment together with human milk and food. Dioxins are well-known for causing cancer, severe reproductive and developmental problems, damage the immune system and for interfering with hormonal systems. Dioxin exposure has further been suggested to induce birth defects, reduced sperm counts, diabetes, learning disabilities, immune system suppression, lung problems, skin disorders, lowered testosterone levels and more. The data originates from national monitoring programs on contaminants financed by the Swedish Environmental Protection Agency (EPA) and accomplished by the Swedish Food Agency (SFA), the Swedish Museum of Natural History (SMNH) and Stockholm University (SU). Temporal trends of the abovementioned chemicals have been studied, also, the trends have been extrapolated in an attempt to forecast the situation during the coming 20 years. The present report focus on temporal trends and longer time series (often more than 2 decades). Compilations that covers also shorter time-series, relations between various biological samples and geographical distribution can be found elsewhere. A thorough study describing the dioxin situation in the Baltic was carried out by the Swedish EPA 2013 (Wiberg et al., 2013).

Naturvårdsverket har under flera decennier, inom den nationella miljöövervakningen, undersökt tidstrender av bioackumulerande/biomagnifierande organiska miljöföroreningar (persistent organic pollutants, POPs) i biota och människor, eftersom POPs kan utgöra hälsorisker för djur och människor. Ett viktigt syfte med detta monitoreringsprogram är att följa miljötillståndet i Sverige. Programmet används också för att följa upp resultat av de åtgärder som vidtagits nationellt och internationellt för att begränsa POP-förororeningen av miljön. I denna rapport undersöks tidstrender av POPs i människor från Sverige (modersmjölk och blodserum), sillgrisslor från Östersjön (ägg) och sill/strömming (muskel och lever) från svenska ost- och västkusten, och dessa trender kopplas samman med de viktigaste nationella/internationella åtgärderna (lagstiftning, råd/rekommendationer, frivilliga åtgärder, mm) som införts för att begränsa utsläppen i miljön. Syftet är att undersöka om det finns samband mellan åtgärder och förändringar av tidstrender i biota och människor. De studerade POPs omfattar industrikemikalierna polyklorerade bifenyler (PCB), de oavsiktligt bildade föroreningarna polyklorerade dibenso-para-dioxiner och dibensofuraner (PCDD/F), fungiciden hexaklorbensen (HCB), de bromerade flamskyddsmedlen (BFR) polybromerade difenyletrar (PBDE) och hexabromcyklododekan (HBCDD), och industrikemikalierna per- och polyfluorerade alkylsubstanser (PFAS). Resultaten visar att nationella/internationella förbud av produktion och användning av PCB och HCB relativt snabbt resulterade i minskande halter i alla studerade matriser. Liknande effekter observerades efter mer eller mindre frivilliga utfasningar av produktion och användning av vissa BFR och PFAS. Halterna av PCDD/F, som förekom som förorening i tekniska PCB-blandningar, minskade också efter att förbud mot PCB-produktion och användning infördes. Detta visar att eliminering av primära källor för utsläpp i miljön är en mycket effektiv åtgärd, som relativt snabbt leder till sjunkande halter i biota och människor även när det gäller så pass svårnedbrytbara substanser som de studerade POPs. När de flesta viktiga primära källorna har eliminerats finns det dock sekundära källor som kan vara mycket svårare, eller helt omöjliga, att eliminera. Detta illustreras av HCB, som för närvarande tycks öka i vissa delar av den svenska miljön. Det har föreslagits att detta fenomen till viss del beror på avdunstning av HCB från förorenad mark i områden som har haft en historiskt högre användning av fungiciden än i Sverige. När det avdunstade HCB med vindarna når Sverige sker en deposition på grund av ett kallare klimat. Diffusa primära källor för PCDD/F, som nu tycks dominera i Sverige, är också svåra att åtgärda, vilket kan förklara varför minskningen av halterna i flera av de studerade matriserna nu verkar gå långsammare än tidigare. Resultaten visar också att stegvis eliminering av produktion och användning av några få substanser i taget inom en grupp av POPs är ineffektivt ur miljömässig synvinkel. Detta exemplifieras av de studerade BFR och PFAS, som i motsats till PCB inte har reglerats gruppvis. Stegvisa åtgärder ger en mycket mer utdragen förbättringsprocess i miljön, där minskande halter av reglerade substanser motverkas av ökande halter av oreglerade substanser med liknande egenskaper. För att undvika denna, ur miljöns synvinkel, utdragna process bör ämnen med liknande egenskaper inom en POP-grupp regleras samtidigt. För vissa av de undersökta POPs har olika delar av den svenska miljön ”svarat” olika snabbt på vidtagna åtgärder. För tetra-pentaBDE vändes en ökning av halter till en minskning mer än 10 år tidigare i sillgrissla och strömming/sill än i modersmjölk. Även om det inte klart går att bevisa, så kan detta bero på att det vidtogs regionala åtgärder i ett tidigt skede som hade positiv effekt på utsläpp i Östersjön utan att nämnvärt påverka den svenska befolkningens exponering. Tidstrenderna i modersmjölk följde istället i hög grad förändringarna i världsproduktion av dessa PBDE. De retrospektiva studierna av BFR och PFAS trender visar att en oreglerad ökning av världsproduktion och -användning har resulterat i exponentiella ökningar av föroreningen av den svenska miljön. Det är därför av yttersta vikt att reglerande myndigheter/organisationer och industrin tillsammans anstränger sig att införa effektiva och snabba åtgärder på global nivå som minimerar risken för framtida miljöproblem orsakade av hittills ”okända” substansgrupper med POP-liknande egenskaper.