Occurrence Of Legacy Research Articles

Occurrence of legacy and emerging organophosphate flame retardants (OPFRs) on silicone wristbands: Comparison within couples

Novel organophosphate flame retardants (OPFRs) are recently identified and highly detected in indoor dusts, but their personal exposure was not clear. Here, wristband was used to estimate non-dietary exposure to emerging OPFRs in comparison with legacy OPFRs in 93 adults in Beijing, China. Comparison of studies in wristband monitoring data showed a clear difference in profiles of legacy OPFRs between China and United States, where tris(1,3-dichloro-2-propyl) phosphate (TDCIPP) was usually the dominant OPFR in the United States, but triphenyl phosphate has the highest contribution to total OPFRs in China. Five emerging OPFRs, including diethylene glycol bis(bis(2-chloroisopropyl) phosphate) (DEGBBCPP) and bis(2-ethylhexyl) phenyl phosphate (BEHPP), were detected in above 45 % of wristbands. The median concentration of DEGBBCPP (2.2 ng/g) was about three times higher than TDCIPP (0.76 ng/g), a legacy chloro-OPFR. Both emerging and legacy OPFRs were significantly correlated within 40 pairs of couples, suggesting major exposure in their homes. Wristbands from husbands had significantly higher tris(2-butoxyethyl) phosphate (TBOEP) and DEGBBCPP, while 2-ethylhexyl diphenyl phosphate (EHDPP) was significantly higher in wives' bands, suggesting gender-related exposure sources for these OPFRs.

Occurrence of legacy and Emerging per- and polyfluoroalkyl substances (PFASs) in indoor dust from office environment in south china

Per- and polyfluoroalkyl substances (PFASs) constitute a broad group of fluorinated organic chemicals that are widely used in consumer products and industrial applications due to their excellent physicochemical properties. Given that people spend a significant portion of their time in office environments, our understanding of the environmental presence and human exposure to these chemicals is crucial. In this study, we conducted a targeted analysis of 24 PFASs in office indoor environments. The ΣPFAS concentrations ranged from 51.6 to 219 ng/g with mean (±SE) and median concentrations of 114 (±5.75) and 107 ng/g, respectively. Hexafluoropropylene oxide dimer acid (HFPO-DA) was the most abundant emerging PFAS detected in the dust, with mean and median concentrations of 40.5 (±1.62) and 40.4 ng/g, respectively, comprising 34.2 % of the ΣPFAS concentrations. Notably, HFPO-DA exhibited a positive correlation with perfluorooctane sulfonate (PFOS) (r: 0.427, p < 0.01), suggesting a potential common source for these two compounds. Our findings underscore the significant contribution of emerging PFASs to total PFAS concentrations and raise concerns about their chronic toxicity and potential health risks to humans in office indoor environments.

Legacy and emerging contaminants in marine mammals from Argentina

Marine mammals are recognized sentinels of ecosystem health. They are susceptible to the accumulation and biomagnification of pollutants, which constitute one of the greatest threats to their survival. Legacy, such as organochlorine pesticides, and emerging contaminants, like microplastics and pharmaceuticals, may have effects on marine mammals' health at individual and population levels. Therefore, the evaluation of the risks associated with pollutants in this group is of great importance. The aim of this review is to provide information on the occurrence of legacy and emerging contaminants in marine mammals that inhabit Argentine waters. Also, to identify knowledge gaps and suggest best practices for future research. Reports of legacy contaminants referring to organochlorine pesticides and polychlorinated biphenyls were found in five species of cetaceans and two of pinnipeds. With respect to emerging pollutants, the presence of plastics was only evaluated in three species. Reported data was from at least a decade ago. Therefore, it is necessary to update existing information and conduct continuous monitoring to assess temporary trends in pollutants. All the studies were carried out in the province of Buenos Aires and Northern Patagonia indicating a knowledge gap in the southern zone of the Argentine Sea. In addition, pollutants of global environmental concern that have not been studied in Argentina are discussed. Future studies should fill these gaps and a greater effort to understand the relationships between pollutants and their effects on marine mammals is suggested. This issue will make it possible to determine thresholds for all the substances and species evaluated in order to carry out more detailed risk assessments and make decisions for the conservation of marine mammals in Argentine waters.

Occurrence of legacy and alternative per- and polyfluoroalkyl substances in serum from high exposure population and their disrupting effects on serum lipids and thyroid function

High exposure of per- and polyfluoroalkyl substances (PFAS) has been reported in main chemical production areas in China, while epidemiological study on exposure risk of PFAS is still limited. In this study, legacy and alternative PFAS were measured in serum samples from 161 adults living in Laizhou Bay, a famous chemical production area located in Shandong province, Northern China. Based on the concentrations of serum PFAS, the disrupting effects of PFAS on serum lipids and thyroid function were further explored. The results showed that the serum perfluorooctanoic acid (PFOA) (geometric mean (GM): 60 ng/mL) in this region was even higher than serum PFOA of residents living in PFOA contaminated water districts in United States and Sweden. 100 % of the serum PFOA was higher than the reference dose for increased total cholesterol (TC). Consistently, higher serum PFOA was marginally correlated with increased TC level (p = 0.062) and low-density lipoprotein (p = 0.065). In addition, higher perfluoroisopropyl perfluorooctanesulfonate and 6:2 chlorinated polyfluoroalkyl ether sulfonates (6,2 Cl-PFESA) were significantly correlated with increased high-density lipoprotein (p = 0.040, 0.022). No significant association was observed between individual PFAS and any thyroid function biomarker. However, using the principal component analysis derived factors to represent the co-exposure patterns, co-exposure of legacy long-chain PFAS showed synergistic effects on the free thyroxine, while the mixture of alternative PFAS showed a synergistic influence on the total and free triiodothyronine.

Presence and inputs of legacy and novel per- and polyfluoroalkyl substances from rivers and drainage outlets to Liaodong Bay, China

Legacy and novel per- and polyfluoroalkyl substance (PFAS) concentrations were measured in 93 water samples from the rivers and drainage outlets to Liaodong Bay, China. The concentrations of Σ19PFASs in river water samples ranged from 7.75 ng/L to 750 ng/L. The concentration ranges for municipal wastewater and industrial wastewater samples were 13.9 to 360 ng/L and 30.6 to 73.1 ng/L, respectively. PFOA was the predominant PFAS along the coast of Liaodong Bay, but PFBA was also present in high concentrations in all samples. For the novel PFAS alternatives, the detection frequencies of 6:2 chlorinated polyfluorinated ether sulfonate (6:2 Cl-PFESA) and hexafluoropropylene oxide dimer acid (HFPO-DA) were 43.0% and 55.9%, respectively. The estimated total discharge of Σ19PFASs reached 1.7 ton/year in rivers and drainage outlets along Liaodong Bay. River water input accounted for 98.6% of the total input, suggesting that it made a major contribution to PFAS pollution in Liaodong Bay. Capsule:The occurrence of legacy and novel per- and polyfluoroalkyl substances from rivers and drainage outlets directly discharging to Liaodong Bay of China was investigated, and their mass discharges were estimated and compared.

Occurrence of legacy and replacement plasticizers, bisphenols, and flame retardants in potable water in Montreal and South Africa

The occurrence of thirty-nine contaminants including plasticizers, bisphenols, and flame retardants in potable water from Montreal and South Africa was analyzed to determine their presence and concentrations in different water sources. In Montreal, five bottled water (BW) brands and three drinking water treatment plants (DWTP) were included. In South Africa, water was sampled from one urban DWTP located in Pretoria, Gauteng, and one rural DWTP located in Vhembe, along with water from the same rural DWTP which had been stored in small and large plastic containers. A combination of legacy compounds, typically with proven toxic effects, and replacement compounds was investigated. Bisphenols, Dechlorane-602, Dechlorane-603, and s-dechlorane plus (s-DP) were not detected in any water samples, and a-dechlorane plus (a-DP) was only detected in one sample from Pretoria at a concentration of 1.09 ng/L. Lower brominated polybrominated diphenyl ethers (PBDE)s were detected more frequently than higher brominated PBDEs, always at low concentrations of <2 ng/L, and total PBDE levels were statistically higher in South Africa than in Montreal. Replacement flame retardants, organophosphate esters (OPEs), were detected at statistically higher concentrations in Montreal's BW (68.56 ng/L), drinking water (DW) (421.45 ng/L) and Vhembe (198.33 ng/L) than legacy PBDEs. Total OPE concentrations did not demonstrate any geographical trend; however, levels were statistically higher in Montreal's DW than Montreal's BW. Plasticizers were frequently detected in all samples, with legacy compounds DEHP, DBP, and replacement DINCH being detected in 100 % of samples with average concentrations ranging from 6.89 ng/L for DEHP in Pretoria to 175.04 ng/L for DINCH in Montreal's DW. Total plasticizer concentrations were higher in Montreal than in South Africa. The replacement plasticizers (DINCH, DINP, DIDA, and DEHA) were detected at similar frequencies and concentrations as legacy plasticizers (DEHP, DEP, DBP, MEHP). For the compounds reported in earlier studies, the concentrations detected in the present study were similar to other locations. These compounds are not currently regulated in drinking water but their frequent detection, especially OPEs and plasticizers, and the presence of replacement compounds at similar or higher levels than their legacy compounds demonstrate the importance of further investigating the prevalence and the ecological or human health effects of these compounds.

Occurrence of Legacy and Emerging Poly- and Perfluoroalkyl Substances in Fluorocarbon Paint and Their Implications for Emissions in China

Occurrence of Legacy and Emerging Poly- and Perfluoroalkyl Substances in Fluorocarbon Paint and Their Implications for Emissions in China

Occurrence of legacy and emerging poly- and perfluoroalkyl substances in water: A case study in Tianjin (China)

Due to the water solubility and environmentally persistent properties of poly- and perfluoroalkyl substances (PFAS), the contamination of PFAS in drinking water is raising widespread concerns for their potential adverse health risks. In the present study, the behavior of PFAS from source waters to effluent water was analyzed by taking samples from three drinking water sources (Yuqiao Reservoir, Beidagang Reservoir, and Yangtze River) and effluent of several treatment processes used in one drinking water treatment plant (DWTP) of Tianjin (China), including pre-chlorination, coagulation, sand filtration, and chlorination. The range of total concentration of PFAS (∑21PFAS) in three source water was 6.64–19.80 ng/L (Yuqiao Reservoir), 80.00–119.86 ng/L (Beidagang Reservoir), and 15.87 ng/L (Yangtze River), respectively. As for individual PFAS, PFBA (perfluorobutanoic acid) was the most abundant PFAS, followed by PFOA (perfluorooctanoic acid), PFBS (perfluorobutane sulfonate), and PFOS (perfluorooctane sulfonate), especially, 6:2 Cl-PFESA (6:2 Cl-polyflurinated ether sulfonate) was detected in all samples. During treatment, the removal rate of ∑21PFAS was 11%, and the removal rate of long-chain PFAS such as PFNA (perfluorononanoic acid), PFOS, and PFDS (perfluorodecane sulfonate) were relatively higher than short-chain PFAS due to their hydrophobic characteristic. Besides, the influence of seasonal factor (precipitation) on the occurrence and composition characteristics of PFAS in the aquatic environment was also investigated, and the results demonstrated that precipitation affected the total concentrations of PFAS in the aquatic environment, but barely on the composition characteristics of PFAS. Furthermore, the ecological risks could be negligible based on the concentration of PFAS measured in surface water. In the meanwhile, the health risks were also assessed based on the concentration of PFAS detected in drinking water, the result indicated that the concentrations of PFAS were less than the suggested drinking water advisories. In addition, more attention should be paid to the risk caused by the frequently detected emerging PFAS such as 6:2 Cl-PFESA and HFPO-DA (hexafluoropropylene oxide-dimer acid).

The Occurrence of Legacy P Soils and Potential Mitigation Practices Using Activated Biochar.

The long-term application of manures in watersheds with dense animal production has increased soil phosphorus (P) concentration, exceeding plant and soil assimilative capacities. The P accumulated in soils that are heavily manured and contain excess extractable soil P concentrations is known as legacy P. Runoff and leaching can transport legacy P to ground water and surface water bodies, contributing to water quality impairment and environmental pollution, such as eutrophication. This review article analyzes and discusses current and innovative management practices for soil legacy P. Specifically, we address the use of biochar as an emerging novel technology that reduces P movement and bioavailability in legacy P soils. We illustrate that properties of biochar can be affected by pyrolysis temperature and by various activating chemical compounds and by-products. Our approach consists of engineering biochars, using an activation process on poultry litter feedstock before pyrolysis to enhance the binding or precipitation of legacy P. Finally, this review article describes previous examples of biochar activation and offers new approaches to the production of biochars with enhanced P sorption capabilities.

Determination and assessment of human dietary intake of per and polyfluoroalkyl substances in retail dairy milk and infant formula from South Africa

Dairy milk and infant formula play important roles in the diet of adolescents, adults and infants, respectively, in the South African population. However, data on the occurrence of legacy and emerging contaminants such as PFAS in these important food sources is lacking. In this study, the concentration of fifteen PFAS were measured in 23 pooled retail dairy milk and 7 pooled infant formulas by means of an ultrahigh performance liquid chromatography tandem mass spectrometric method. The concentrations of Σ15PFAS ranged from 0.08–15.51 ng mL−1 and 0.42–5.74 ng mL−1 in dairy milk and infant formulas, respectively. PFBA, PFPeA, PFuDA, PFTrDA and PFDoA were the most prevalent PFAS in both matrices with detection frequency > 96%. Highest PFAS concentrations of 2.02 ng ml−1 and 2.76 ng ml−1 were recorded for PFDoA in infant formulas and dairy milk, respectively. The concentrations of legacy PFAS –PFOA and PFOS, shows resemblance with global data, however, elevated concentrations of long chain C9 – C14 PFAS were observed in this study. Though, higher concentrations of PFAS were measured in full cream dairy milk, no statistical significant difference (P = 0.546) was observed for the various classes of dairy milk. The EDI of Σ15PFAS through infant formulas were 184.92, 329.47 and 166 ngkg−1BWday−1 for partially breastfed, exclusively formula fed and older infants, respectively. Similarly, the EDI of PFAS through dairy milk for toddlers, adolescents, female and male adults for the rural population were 14.17, 1.09, 2.59 and 3.16 ngkg−1BWday−1 respectively while they were 20.41, 3.84, 4.13 and 4.26 ngkg−1BWday−1 respectively in the urban population. Although, the EDI of PFAS through the consumption of infant formulas and dairy milk are lower than the daily tolerable limits, the relative importance of long-term exposure and the cumulative effects of multiple exposure pathways cannot be overemphasized.

Occurrence of legacy and emerging organic contaminants in snow at Dome C in the Antarctic

Concentrations of 9 organophosphate esters (OPEs), 16 perfluoroalkylated substances (PFASs) and 17 polycyclic aromatic hydrocarbons (PAHs) were investigated in surface snow samples collected at Dome C on the Antarctic Plateau in summer 2016. Tris(1-chloro-2-propyl) phosphate (TCPP), tris-(2-chloroethyl) phosphate (TCEP) and tri-n-butylphosphate (TnBP) were the dominant compounds of OPEs, with mean concentrations of 8157 ± 4860, 1128 ± 928 and 1232 ± 1147 pg/L. Perfluorooctanoic acid (PFOA, mean: 358 ± 71 pg/L) was the dominant compound of PFASs, and following by perfluoro-n-hexanoic acid (PFHxA, mean: 222 ± 97 pg/L), perfluoro-n-heptanoic acid (PFHpA, 183 ± 60 pg/L) and perfluoro-n-pentanoic acid (PFPeA, 175 ± 105 pg/L). 2-(Heptafluoropropoxy)propanoic acid (HFPO-DA, mean: 9.2 ± 2.6 pg/L) was determined in the Antarctic for the first time. Significantly positive correlations were observed between HFPO-DA and the short-chain PFASs, implying they have similar emission sources and long-range transport potential. High levels of 2-methylnaphthalene and 1-methylnaphthalene, as well as the ratios of PAH congeners indicated PAHs were attributable mostly to combustion origin. Occurrence and profiles of the indicators of OPEs, PFASs and PAHs, as well as air mass back-trajectory analysis provided direct evidences of human activities on Concordia station and posed obvious impacts on local environments in the Antarctic. Nevertheless, the exchange processes among different environmental matrices may drive the long-range transport and redistribution of the legacy and emerging Organic contaminants from coast to inland in the Antarctic.

Novel and legacy per- and polyfluoroalkyl substances (PFASs) in a farmland environment: Soil distribution and biomonitoring with plant leaves and locusts

The occurrence of legacy and novel per- and polyfluoroalkyl substances (PFASs) in multiple matrices from a farmland environment was investigated in the Beijing-Tianjin-Hebei core area of northern China. PFASs were ubiquitously detected in farmland soils, and the detection frequency of 6:2 chlorinated polyfluoroalkyl ether sulfonic acid (6:2 Cl-PFESA) was higher than that of perfluorooctane sulfonic acid (98% vs. 83%). Long-chain PFASs, including 6:2 Cl-PFESA, showed a centered distribution pattern around the metropolis of Tianjin, probably due to the local intensive industrial activity, while trifluoroacetic acid (TFA) showed a decreasing trend from the coast to the inland area. Other than soil, TFA was also found at higher levels than other longer-chain PFASs in dust, maize (Zea mays), poplar (Populus alba) leaf and locust (Locusta migratoria manilens) samples. Both poplar leaves and locusts can be used as promising biomonitoring targets for PFASs in farmland environments, and their accumulation potential corresponds with protein and lipid contents. Apart from being exposed to PFASs via food intake, locusts were likely exposed via uptake from soil and precipitated dust in farmland environments. The biomonitoring of locusts may be more relevant to insectivores, which is important to conducting a comprehensive ecological risk assessment of farmland environments.

Occurrence of legacy and emerging organic pollutants in whitemouth croakers from Southeastern Brazil

The whitemouth croaker (Micropogonias furnieri) is one of the most commercially important species along the Atlantic coast of South America. Moreover, some of its biological traits (long life span, inshore feeding, high trophic position) make this species a suitable sentinel of coastal pollution. Here, we investigated contamination by multiple legacy and emerging organic pollutants, such as brominated and chlorinated flame retardants, polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs), in whitemouth croakers from two estuaries (Guanabara and Sepetiba Bays) located in industrialized and urbanized areas in Rio de Janeiro State, Southeastern Brazil. Furthermore, we assessed how biological and ecological features could explain the observed contamination patterns. Regarding brominated flame retardants, concentrations of polybrominated diphenyl ethers (PBDEs) varied from 7.6 to 879.7 pg g−1 wet weight (w.w.), with high contribution of tetra-, penta-, hexa- and deca-BDEs. The sum of chlorinated flame retardants (dechlorane-related compounds, ΣDRC) ranged from <LOD to 41.1 pg g−1 w.w., mostly represented by Dechlorane 603 and Dechlorane Plus (DP). Concentrations of PCDDs and PCDFs varied from <LOD to 1.7 pg g−1 w.w., while the Toxic Equivalent (TEQ-PCDD/Fs) levels ranged from 0.1 to 0.2 pg g−1 w.w. Positive correlations between δ15N and concentrations of tri-, tetra- and penta-BDEs, as well as ΣDRC, DP and anti-DP isomers suggested that ecological factors (namely biomagnification along the food web) influence contamination of whitemouth croakers in the estuaries studied. Moreover, the sum of PBDEs (ΣPBDE), tri- and tetra-BDEs concentrations were negatively correlated with fish size, suggesting that depuration by fishes and/or habitat shift throughout the whitemouth croaker's life cycle might also influence concentrations. Overall, our study emphasized the need for further investigations to help understand the complex patterns of bioaccumulation and biomagnification that seem to exist in Southeastern Brazil.

Occurrence of legacy and alternative plasticizers in indoor dust from various EU countries and implications for human exposure via dust ingestion and dermal absorption

Plasticizers are a category of chemicals extensively used in consumer products and, consequently, their presence is ubiquitous in the indoor environment. In the present study, an analytical method has been developed for the quantification of plasticizers (7 legacy phthalate esters (LPEs) and 14 alternative plasticizers (APs)) in indoor floor dust based on ultrasonic and vortex extraction, Florisil fractionation and GC-(EI)-MS analysis. Dust samples (n = 54) were collected from homes, offices, and daycare centers from different EU countries (Belgium, the Netherlands, Ireland and Sweden). Method LOQs ranged from 0.2 to 5 μg/g. Tri-n-hexyl trimellitate (THTM) was not detected in any sample, whereas dimethyl phthalate (DMP), diphenyl phthalate and acetyl triethyl citrate (ATEC) were detected only in 6, 2 and 1 out of 54 samples, respectively. The highest concentrations of plasticizers were measured in Swedish offices, at a mean concentration of total plasticizers of 1800 μg/g, followed by Swedish daycare centers at 1200 and 670 μg/g for winter and spring sampling, respectively. Generally, the contribution of APs was slightly higher than for LPEs for all indoor environments (mean contribution 60% and 40%, respectively based on contributions per indoor environment). For the APs, main contributors were DINP in Belgian homes (28%), Swedish offices (60%), Swedish daycare centers (48%), and Dutch offices (31%) and DEHT in Belgian (28%), Irish (40%) and Dutch homes (37%) of total APs. The predominant LPE was bis-2-ethylhexyl-phthalate (DEHP) with a mean contribution varying from 60% to 85% of total LPEs. Human exposure was evaluated for dust ingestion and dermal absorption using hazard quotients (HQs) of plasticizers (ratio between average daily doses and the reference dose). None of the HQs of plasticizers exceeded 1, meaning that the risk for adverse human health effects from these plasticizers via dust ingestion and dermal absorption is unlikely.

Occurrence of Legacy and New Persistent Organic Pollutants in Avian Tissues from King George Island, Antarctica.

Legacy and new persistent organic pollutants (POPs), including polychlorinated naphthalenes (PCNs), Dechlorane Plus (DPs) and related compounds (Dechloranes), hexabromocyclododecanes (HBCDs), polychlorinated biphenyls (PCBs), and organochlorine pesticides (OCPs), were analyzed in avian tissue samples from King George Island, Antarctica. The avian species consisted of the Gentoo penguin (Pygoscelis papua), the Adelie penguin (Pygoscelis adeliae), the South polar skua (Stercorarius maccormicki), and the Brown skua (Stercorarius antarcticus). HBCDs were detected in all samples and ranged from 1.67-713 pg/g-lipid. In the penguin samples, the concentrations of PCNs ranged from 0.69-2.07 ng/g-lipid, whereas those in the skua samples ranged from 7.41-175 ng/g-lipid. The levels of Dechloranes ranged from 0.60-1.30 ng/g-lipid in the penguin samples and from 6.57-47.4 ng/g-lipid in the skua samples. The concentrations and congener distributions of OCPs and PCBs were similar to the results of previous reports. The three new POPs were detected in all samples, and this study was one of the first reports on the occurrence of these pollutants in the Antarctic biota. Because Antarctica is one of the most pristine places on Earth, the detection of new POPs in the Antarctic birds, especially penguins, is direct evidence of the long-range transport of pollutants. Furthermore, the concentration ratios of the penguin to the skua samples (BMFs-p) were greater than 1 in most legacy and new POPs, and the BMFs-p values of the new POPs were comparable to those of some OCPs, suggesting a possibility of biomagnification. Despite the small sample size, the results of this study identified POP contamination of the Antarctic avian species and long-range transport and biomagnification of HBCDs, Dechloranes, and PCNs.

Occurrence of legacy and emerging halogenated organic contaminants in marine shellfish along French coasts

Current contamination levels of selected legacy, currently-used and emerging halogenated contaminants were monitored in marine shellfish along French coastlines. The studied contaminants included polybrominated diphenyl ethers (PBDEs), hexabromocyclododecanes (HBCDDs), 1,2-bis(2,4,6-tribromophenoxy)ethane (BTBPE), decabromodiphenylethane (DBDPE), hexabromobenzene (HBB), 2,2′,4,4′,5,5′-hexabromobiphenyl (BB-153) and perfluorinated compounds (PFCs).BDE-47, BDE-209, BTBPE, HBB and α-HBCDD were detected in 100% of the analyzed samples, whereas BB-153, DBDPE and PFOS were detected at frequencies of 97%, 90% and 55%, respectively. Concentrations were in the pgg−1ww range and varied as follows: PFOS>BDE-47∼α-HBCDD>BDE-209>BTBPE∼DBDPE>HBB∼BB-153. Overall, non-PBDE Brominated Flame Retardants (BFRs) revealed concentrations between 3 and 59 times lower than those of PBDEs.PBDE pattern was dominated by BDE-47, followed by BDE-99>BDE-100>BDE-49>BDE-209>BDE-154; these 6 congeners represented 94% of the summed ten PBDEs. PFC pattern determination revealed PFOS as the predominant PFC in samples from the English Channel and Atlantic, whereas perfluorocarboxylic acids (PFCAs) prevailed in Mediterranean samples. Temporal trend investigations on archived samples from the Mediterranean coast collected between 1981 and 2012 showed a prevalence of PFOS until 1998; PFCAs subsequently increased and became more abundant than PFOS. High levels of PFCAs were observed until 2008, followed by a decrease and stabilization in 2010–2012. Amongst PFCAs, perfluorotridecanoic acid (PFTrDA) and perfluoroundecanoic acid (PFUnA) were predominant and exhibited similar time trends, suggesting similar sources at the investigated site, home to major industrial activity.