Perfluorinated alkyl substances in water, sediment, plankton and fish from Korean rivers and lakes: A nationwide survey

Science of the Total Environment xxx (2014) xxx–xxx

STOTEN-15762; No of Pages 9

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Science of the Total Environment

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Perfluorinated alkyl substances in water, sediment, plankton and fishfrom Korean rivers and lakes: A nationwide survey

Nguyen-Hoang Lam a, Chon-Rae Cho b, Jung-Sick Lee a, Ho-Young Soh a, Byoung-Cheun Lee c, Jae-An Lee c,Norihisa Tatarozako d, Kazuaki Sasaki e, Norimitsu Saito e, Katsumi Iwabuchi e,Kurunthachalam Kannan f, Hyeon-Seo Cho a,⁎a College of Fisheries and Ocean Sciences, Chonnam National University, Yeosu 550-749, Republic of Koreab Korea Research Institute of Chemical Technology, Daejeon 305-600, Republic of Koreac National Institute of Environmental Research, Incheon 404-408, Republic of Koread National Institute for Environmental Studies, Tsukuba, Ibaraki 305-8506, Japane Research Institute for Environmental Sciences and Public Health of Iwate Prefecture, Iwate 020-0852, Japanf Wadsworth Center, New York State Department of Health, and School of Public Health, State University of New York at Albany, Empire State Plaza, PO Box 509, Albany, NY 12201-0509, USA

H I G H L I G H T S

• PFOS was found at greatest concentrations in water, sediment, plankton and fish.• High concentrations of long chain PFCAs were found in sediment samples.• Mean ratios of PFASs concentration in fish blood to liver were mostly N2.• PFOS, PFUnA, PFDoA and PFDA accounted for 94–99% of ∑PFASs concentration in fish.• Only PFOS and PFNA were concentrated in plankton samples.

⁎ Corresponding author. Tel.: +82 616597146; fax: +8E-mail address: [email protected] (H.-S. Cho).

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Please cite this article as: Lam N-H, et al, Pernationwide survey, Sci Total Environ (2014)

a b s t r a c t
a r t i c l e i n f o
Article history:Received 30 October 2013Received in revised form 10 January 2014Accepted 10 January 2014Available online xxxx

Keywords:PerfluorooctanesulfonatePerfluorinated compoundsKoreaFreshwaterBioconcentration factorFish tissues

Water, sediment, plankton, and blood and liver tissues of crucian carp (Carassius auratus) and mandarin fish(Siniperca scherzeri)were collected from sixmajor rivers and lakes in South Korea (includingNamhanRiver, BukhanRiver, Nakdong River, NamRiver, Yeongsan River and Sangsa Lake) and analyzed for perfluorinated alkyl substances(PFASs). Perfluorooctane sulfonate (PFOS)was consistently detected at the greatest concentrations in all media sur-veyed with the maximum concentration in water of 15 ng L−1 and in biota of 234 ng mL−1 (fish blood). A generalascending order of PFAS concentration of water b sediment b plankton b crucian carp tissues b mandarin fish tis-sues was found. Except for the Nakdong River and Yeongsan River, the sum PFAS concentrations in water sampleswere below 10 ng L−1. The PFOS and perfluorooctanoic acid (PFOA) concentrations in water did not exceed levelsfor acute and/or chronic effects in aquatic organisms. High concentrations of long chain perfluorocarboxylates(LCPFCAs) were found in sediment samples. PFOS, perfluoroundecanoic acid (PFUnA), perfluorododecanoic acid(PFDoA) and perfluorodecanoic acid (PFDA) accounted for 94–99% of the total PFASs concentration in fish tissues.The mean ratios of PFAS concentration between fish blood and fish liver were above 2 suggesting higher levels inblood than in liver. Significant positive correlations (r N 0.80, p b 0.001)were observed betweenPFOS concentrationin blood and liver tissues of both crucian carp andmandarinfish. This result suggests that blood can be used for non-lethal monitoring of PFOS in fish. Overall, the rank order of mean bioconcentration factors (BCFs) of PFOS in biotawas; phytoplankton (196 L/kg) b zooplankton (3233 L/kg) b crucian carp liver (4567 L/kg) b crucian carp blood(11,167 L/kg) b mandarin liver (24,718 L/kg) b mandarin blood (73,612 L/kg).

© 2014 Elsevier B.V. All rights reserved.

1. Introduction

The unique properties such as resistance to hydrolysis, photolysis,bio-degradation and thermal stability, in combination with widespread

2 61 654 2975.

ghts reserved.

fluorinated alkyl substances i, http://dx.doi.org/10.1016/j.s

application of perfluoroalkyl substances (PFASs),made themglobal pol-lutants in abiotic and biotic matrices including food stuffs (Picó et al.,2011), human blood (Kannan et al., 2004; Harada et al., 2010), breastmilk (Llorca et al., 2010), wildlife such as fish, birds and marine mam-mals (Giesy and Kannan, 2001), sediment (Nakata et al., 2006), water(Yamashita et al., 2005) and atmosphere (Li et al., 2011). Theworldwidedistribution of PFASs was reported in urban and remote areas including

n water, sediment, plankton and fish from Korean rivers and lakes: Acitotenv.2014.01.045

http://dx.doi.org/10.1016/j.scitotenv.2014.01.045

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Fig. 1. Map showing 17 sampling sites located in six major rivers and lakes from SouthKorea.

2 N.-H. Lam et al. / Science of the Total Environment xxx (2014) xxx–xxx

deep oceanicwater of up to 5000m (Yamashita et al., 2005) and in polarbears from the Arctic Ocean (Giesy and Kannan, 2001).

Due to their persistence and bioaccumulation, some PFASs canelicit harmful effects in terrestrial and aquatic organisms (Lau et al.,2004). Perfluorooctane sulfonate (PFOS) also biomagnifies in wildlifeat higher trophic levels in the food chain (Giesy and Kannan, 2001;Kannan et al., 2005). To humans, the major routes of PFAS exposuresinclude diet (Tittlemier et al., 2007; Zhang et al., 2010), drinkingwater (Takagi et al., 2008; Nolan et al., 2010; Llorca et al., 2012)and indoor dust (Strynar and Lindstrom, 2008; Björklund et al.,2009).

Following the discovery of widespread global contamination byPFOS, the 3 M Company, a major producer of this compound, phasedout its production in the USA from 2001 (Giesy and Kannan, 2001). Sev-eral other countries have put forward some regulations to ban or limitthe use of PFASs; for example, in industrial and domestic products inCanada and European Union in 2006. PFOS and, its salts andperfluorooctane sulfonyl fluoride were listed on Annex B of TheStockholm Convention on persistent organic pollutants by the FourthConference of Parties in May 2009 (Kannan, 2011).

South Korea is a developed and industrialized country. PFASs havebeen used extensively in various industries including electronic and tex-tile industries in South Korea. The concentrations of PFASs in surfacewater from certain industrial areas in South Korea are the highestamong several Asian countries as well as globally (Rostkowski et al.,2006; Cho et al., 2010). Previous studies have also reported high accu-mulation of PFASs in human blood (Kannan et al., 2004; Harada et al.,2010; Ji et al., 2012), birds (Kannan et al., 2002a; Yoo et al., 2008),minke whales and common dolphins (Moon et al., 2010), Asian peri-winkles and rockfish (Naile et al., 2010) and coastal and ocean watersfrom Korea (So et al., 2004; Yamashita et al., 2005; Rostkowski et al.,2006; Naile et al., 2010). Despite this, available studies on PFASs in Ko-rean freshwater ecosystems such as lakes or rivers are limited. Here,we carried out a systematic study during 2010 to 2012 to determinethe current status and extent of PFAS concentrations in both abioticand biotic matrices in six major rivers and lakes in Korea. Rivers andlakes were surveyed along a spatial gradient representing upstreamand downstream locations to identify sources of pollution. Accumula-tion in tissues (blood and liver) of various freshwater aquatic organismswas investigated.

2. Materials and methods

2.1. Chemicals and reagents

MPFAC-MXA, a mixture of 9 surrogate standards containing 13C4-PFOS (sodium perfluoro-1-[1,2,3,4-13C4] octane sulfonate), and 13C4-PFOA (Perfluoro-n-[1,2,3,4-13C4]) octanoic acid were purchased withPFAC-MXB, a mixture of 17 native perfluorocarboxylate acids (PFCAs)and perfluoroalkyl sulfonates from Wellington Laboratories (Guelph,ON, Canada). 13C4-PFOS was used as a surrogate for the perfluoroalkylsulfonates and 13C4-PFOA was used as a surrogate for the PFCAs. PFAC-MXBmixture was used for standard calibration at concentrations rang-ing from 0.1 to 50 ng/mL. High performance liquid chromatography(HPLC) grade reagents including methanol (Kanto Chemical, Tokyo,Japan), water (J.T Baker, USA) and ammonium acetate (Junsei, Japan)were used. Milli-Q water was prepared by a Barnstead Nanopure Infin-ity TM water purification system (Thermo Scientific, USA).

2.2. Sample collection

Samples of water, sediment, plankton, and blood and liver tissues ofan omnivorousfish species (crucian carp) and a carnivorousfish species(mandarin fish) were collected from 17 sampling sites in six major riv-ers and lakes in South Korea includingBukhan, Namhan,Nakdong, Nam,Yeongsan Rivers and Sangsa Lake (Fig. 1). The Nakdong River, Yeongsan

Please cite this article as: Lam N-H, et al, Perfluorinated alkyl substances inationwide survey, Sci Total Environ (2014), http://dx.doi.org/10.1016/j.s

River and Han River are three of four largest river basins in South Koreaand play an important role as a water resource for agriculture, industry,recreational and drinking water for millions of people living in metro-politan cities of Seoul, Daegu, Busan and Gwangju. The Bukhan andNamhan Rivers are twomajor tributaries of the Han River. The NakdongRiver, and its main tributary, Nam River are located in the southeasternregion; the Yeongsan River and Sangsa Lake are located in the south-western region and the Namhan and Bukhan Rivers are located in thenortheastern region of the Korean peninsula. The sampling areas weredivided generally into 3 groups as highly industrialized areas (YeongsanRiver and Nakdong River), moderately industrialized areas (NamhanRiver and Nam River) and less industrialized areas (Sangsa Lake andBukhan River). In order to survey the effects of discharge of wastewater treatment plant (WWTP) effluents on PFASs concentration in sur-face water samples, the sampling sites 7 and 13were from downstreamof industrial waste water treatment plants (I-WWTP) in Daegu metro-politan city (treatment capacity of 520,000 ton/day) and in Hamantown (treatment capacity of 3400 ton/day), respectively; the samplingsites 16 and 13 were located downstream of domestic waste watertreatment plants (D-WWTP) in Gwangju metropolitan city (treatmentcapacity of 600,000 ton/day) and in Seungju town (capacity of2500 ton/day), respectively. Because the sampling sites were selectedto represent Korea, and involved various levels of industrialization, theresults of this study represent PFAS concentrations in freshwater eco-systems in Korea.

One liter clean polypropylene (PP) bottles pre-rinsed with Milli-Qwater,methanol andwater froma specific sampling sitewere sunk to col-lect surface waters. Surface layer (1–5 cm) of sediment samples was col-lected using a clean,methanol rinsed PP spatula and stored in pre-cleaned50 mL PP tubes. Phytoplankton, micro-zooplankton and meso-zooplankton samples were collected vertically by using NORPAC® plank-ton net with 3 mesh sizes of 20, 60, 200 μm, respectively. Depending onthe depth of water column and topography of fishing sites, fish sampleswere collected by drift gill net, cast net or fish and hook. Fresh bloodand liver tissues were obtained from fish. Sexes, body weight, bodylength, hepatosomatic index (HSI) and gonadosomatic index (GSI) offishes were also determined. Water and sediment samples weretransported on ice, to the laboratory, and keep at 4 °C until extraction.Biota samples were stored in dry ice immediately after collection in thefield and kept at−20 °C in the laboratory until extraction.



3N.-H. Lam et al. / Science of the Total Environment xxx (2014) xxx–xxx

2.3. Sample extraction and analysis

Ten perfluorinated compounds including perfluorohexanoic acid(PFHxA), perfluoroheptanoic acid (PFHpA), perfluorooctanoic acid(PFOA), perfluorononanoic acid (PFNA), perfluorodecanoic acid (PFDA),perfluoroundecanoic acid (PFUnA), perfluorododecanoic acid (PFDoA),perfluorohexane sulfonate (PFHxS), perfluorooctane sulfonate (PFOS),and perfluorodecane sulfonate (PFDS) were the target analytes in thepresent study.

Water samples were not filtered to avoid the loss of some PFASs andpotential for contamination of target PFASs from filter papers during thefiltration procedure. Thus, concentrations reported for water samplesrepresent both dissolved and particulate phase concentrations. Sedi-ment samples were air-dried, crushed with pestle and mortar andsieved through a 0.25 mm sieve prior to extraction. Water sampleswere analyzed following the method described by Yamashita et al.(2004). Sediment samples were extracted based on the method ofNakata et al. (2006). Biota sampleswere analyzed by ion-pair extractionmethod described elsewhere (Hansen et al., 2001; Giesy and Kannan,2001; Hart et al., 2008). Concentrations of PFASs were determined byan Agilent 1100TM HPLC interfaced with Applied Biosystems API2000TM electrospray ionization tandem mass spectrometer (ESI-MS/MS). Ten μL aliquot of the extracted sample were injected. Flow rate ofthe mobile phase was 300 μL/min. To quantify the target chemicals byMS/MS, a multiple reaction monitoring (MRM) mode was used.

2.4. Quality assurance and quality control

Procedural blanks were prepared to check for possible contamina-tions arising from the sample preparation procedure. Concentrationsof target chemicals were subtracted from concentrations found inblanks, when applicable. The regression coefficient (r2) of the calibra-tion curves for all target analytes, prepared at concentrations of 0.1,0.2, 0.5, 1, 2, 5, 10, 20, and 50 ng/mL was ≥0.99. The detection limitsof PFASs in samples ranged from 0.01 to 0.1 ng L−1 for water, 0.01 to0.02 ng g−1 dry weight (dw) for sediment, and 0.01 to 0.1 ng g−1 wetweight (ww) or ng mL−1for biota. The recovery rates (%) of surrogatestandards spiked into each sample prior to extraction were in therange of 73.6% to 131%. The concentrations of target analytes were notcorrected for surrogate recovery rates.

2.5. Statistical analysis

In this study, the parametric method of regression on order statisticsfunction and the nonparametric method of Kaplan–Meier built in thestatistical software of ProUCL 4.1 (U.S. Environmental Protection

Table 1Overview of PFASs analysis results.

Item Water Sediment Plankton

Sampling site (n)a 17 17 2b

Analyzed sample (n) 19 27 12Detected sample n (%) n (%) n (%)PFHxA 15 (79) 6 (22) 0 (0)PFHpA 16 (84) 3 (11) 0 (0)PFOA 17 (89) 24 (89) 0 (0)PFNA 16 (84) 24 (89) 10 (83)PFDA 12 (63) 24 (89) 1 (8)PFUnA 15 (79) 23 (85) 6 (50)PFDoA 12 (63) 27 (100) 7 (58)PFHxS 18 (95) 9 (33) 0 (0)PFOS 19 (100) 27 (100) 6 (50)PFDS 0 (0) 0 (0) 0 (0)Average detected 14 (74) 17 (62) 3 (25)

a Sites 4 and 5 were surveyed in 2010 and others were surveyed in 2012.b Collected in sites 4 and 5.c Collected in sites 2, 4, 5, 7, 10, 13 and 16.


Agency) were utilized to treat the data sets with 0% b % non-detected(NDs) b 80%. Alternatively, if the %NDs in a data set exceeded 80% or ifthe number of distinct observation in a data set was smaller than 5,which is the minimum distinct observation size required to run ProUCL4.1, all NDs were assigned a value of zero (Singh et al., 2006).Spearman's correlation analysis and Student's t-test were also per-formed by using SPSS® (IBM, version 21) to investigate correlationsand statistical differences between selected data groups.

3. Results and discussion

The overall observation of all target analytes in various matrices ispresented in Table 1.

3.1. PFASs in water

Except for the Nakdong River and Yeongsan River, the sum PFASconcentrations in water samples collected in rivers and lakes fromKorea were below 10 ng L−1 (Fig. 2). Among PFASs analyzed, PFOAand PFOS were consistently detected at high concentrations in riverand lake water samples (Table 2). The mean percentages of PFOA andPFOS concentrations in total PFASs concentration in water were 24%and 37%, respectively. The greatest concentrations of PFOA and PFOSwere found in the sampling sites 7 and 16, respectively, which are locat-ed downstream of industrial and domestic waste water treatmentplants (WWTPs) in Daegu and Gwangju metropolitan cities. These re-sults suggest thatWWTPs are the “point-sources” of aqueous dischargesof PFASs into the aquatic environments. The ratios of concentration ofPFOS to PFOA were in the range of 0.23 to 39 (mean = 4.15), which iscomparable to a general concentration ratio of PFOS to PFOA (mean ofN4) in water samples from Korean coastal waters (Naile et al., 2010).Apart from the Nam River, where this ratio ranged from 0.23 to 0.30,the PFOS/PFOA concentration ratio in water samples from other fresh-water sampling sites was generally greater than 1. This result suggeststhat except for the Nam River where PFOA was the dominant PFAS,PFOS was dominant in water samples from the other sampling areas.

Higher concentrations of PFOS and PFOA have been reported in sur-facewaters from some other regions in South Korea andAsia, than thosefound in the present study. In South Korea, the greatest concentrationsof PFOS and PFOA were found in water samples collected from theheavily industrialized area of Shihwa Lake. High concentrations ofPFOS and PFOA in water samples from this “hotspot” were reportedby Rostkowski et al. (2006) (max. PFOS = 651 ng L−1; max. PFOA =61.7 ng L−1; n = 21); Naile et al. (2010) (max. PFOS = 450 ng L−1;max. PFOA = 68.6 ng L−1; n = 8) and So et al. (2004) (mean PFOS =730 ng L−1; mean PFOA = 320 ng L−1; n = 1). Additionally, mean

Carp blood Carp liver Mandarin blood Mandarin liver

7c 7c 2b 2b

69 69 20 20n (%) n (%) n (%) n (%)7 (10) 0 (0) 0 (0) 0 (0)0 (0) 0 (0) 0 (0) 0 (0)24 (35) 9 (13) 19 (95) 9 (45)16 (23) 30 (43) 16 (80) 0 (0)69 (100) 69 (100) 19 (95) 2 (10)69 (100) 69 (100) 20 (100) 20 (100)69 (100) 67 (97) 20 (100) 15 (75)29 (42) 4 (6) 0 (0) 0 (0)69 (100) 58 (84) 20 (100) 20 (100)1 (1) 9 (13) 18 (90) 0 (0)35 (51) 32 (46) 13 (66) 7 (33)



0

10

20

30

40

Bukhan Namhan Nakdong Nam Sangsa Yeongsan

Con

cent

ratio

n (n

g/L

)

River name

mean

min

Q3

median

Q1

max

Fig. 2. SumPFASs concentrations inwater collected from6major rivers and lakes in Korea.The mean total PFAS concentrations in Bukhan River, Namhan River, Nam River andSangsa Lake were below 10 ng/L.


concentrations of PFOS (67.2 ng L−1) and PFOA (32.5 ng L−1) in seawa-ter samples (n=11) fromKoreanWestern and Southern coast reportedby So et al. (2004) were higher than those found in freshwater in thisstudy. In Japan, mean PFOS concentrations in water samples (n = 14)collected from Tokyo Bay, Osaka Bay and Ariake Bay (Taniyasu et al.,2003) were 1.2–6.7 fold greater than the mean PFOS concentrationfound in the present investigation. Senthilkumar et al. (2007) and Lienet al. (2008) also reported higher PFOS and PFOA concentrations inriver water from Kyoto area and the Yodo River basin in Japan thanthose found in the present study, but the concentrations were similarto those reported by Sinclair et al. (2006) for river and lake waters inNewYork (USA), So et al. (2007) forwaters from the Pearl River, Guang-zhou and the Yangtze Rivers, Shanghai (China) and Liu et al. (2009) forrain and snow from Dailan (China). More detailed comparisons of PFOSand PFOA concentration obtained in water samples from the presentstudy with those reported in previous studies are provided in the Sup-plementary information.

PFHxS, PFNA and PFHxA accounted for 12.3%, 6.93% and 6.79% oftotal PFAS concentrations in water samples, respectively. Concentra-tions of these compounds in water samples in the present study wererelatively lower than those reported from the west coast of Korea(Naile et al., 2010) and from Shihwa Lake (Rostkowski et al., 2006)but higher than those reported in water samples from Geonggi Bay(Rostkowski et al., 2006). PFDS was not found in any of water samples,

Table 2Concentration (ng L−1) of PFASs in water showed in min–max (mean).

Site (n) PFHxA PFHpA PFOA PFNA PFDA

Bukhan (3) 0.11–0.31(0.18)

0.12–0.27(0.19)

0.56–1.41(0.94)

0.29–0.52(0.38)

0.10–0.21(0.14)

Namhan (4) ND ND–0.45(0.26)

ND–0.64(0.20)

ND–0.32(0.08)

ND–0.11(0.02)

Nakdong (3) 0.51–7.94(3.82)

0.71–3.43(1.85)

3.56–8.34(6.50)

0.83–4.49(2.32)

0.53–4.80(2.13)

Nam (3) 0.86–1.31(1.03)

0.45–0.91(0.68)

3.40–4.65(3.84)

0.53–0.69(0.62)

0.19–0.33(0.26)

Sangsa (3) 0.02–0.18(0.10)

ND–0.18(0.06)

0.29–0.63(0.43)

0.14–0.33(0.21)

0.05–0.07(0.06)

Yeongsan (3) 0.93–1.33(1.11)

0.41–0.79(0.60)

2.43–4.66(3.97)

0.54–1.08(0.85)

0.14–1.10(0.64)

All sampling sites(19)

ND–7.94(0.98)

ND–3.43(0.59)

ND–8.34(2.49)

ND–4.49(0.71)

ND–4.80(0.52)

n: number of analyzed sample; ND: below the method detection limit.a ∑PFASs refer to sum of ten detectable PFAS in each sampling site.


even in downstream sampling sites of domestic and industrial WWTPsin the Nakdong River (no. 7), Yeongsan River (no.16), Sangsa Lake(no.17) and Nam River (no.13). This is similar with those described inNaile et al. (2010), who reported belowmethod detection limit concen-trations for PFDA in the Yeongsan River estuary, the heavily industrial-ized area of Shihwa Lake and Sinduri Beach. The different patterns ofconcentration of PFASs analyzed in the present study, combined withthe comparisons with other previous studies, suggest a site-specificPFAS sources in Korean surface waters. Thus, further investigations areneeded to identify the sources of PFASs.

The US EPA's Great Lakes Initiative (GLI, USEPA, 1995) intends toprovide both acute and chronic data for the protection of fish, inverte-brates, and other aquatic organisms based on the results of toxicity test-ing with freshwater organisms. In this guideline, acute toxicity datafrom a range of specified taxa was collected to identify a final acutevalue (FAV) that can protect 95% of test species and the acute criterionor criteria maximum concentration (CMC) was established as equiva-lent to one-half of the FAV. Additionally, within the guideline, thechronic criterion or criteria continuous concentration (CCC) wasestablished to represent a concentration of a chemical such that 95%of the genera tested have greater chronic values. Following this guide-line, Giesy et al. (2010) used data from acceptable tests with freshwaterorganisms from North America including a variety of genera such aswater flea, mussel, spring peeper, planarian, amphipod, rainbow trout,leopard frog, oligochaete, fathead minnow, midge and some sensitiveaquatic plants and algae to summarize numerical water quality criteriavalues for selected PFASs. These water quality criteria values were de-termined as 5.1 μg PFOS/L and 2.9 mg PFOA/L for CCC and 21 μg PFOS/L and 25 mg PFOA/L for CMC. An evaluation of potential ecologicalrisks to aquatic organisms associated with exposure to PFOS and PFOAwas employed by comparing the determined concentration of PFOSand PFOA in water samples in the present study with the water qualitycriteria values for the protection of aquatic organisms reported by Giesyet al. (2010). The comparison indicates that PFOS concentrations (up to15.1 ng L−1) and PFOA concentrations (up to 8.34 ng L−1) found in sur-face water samples in the present study were 300–300,000 fold lessthan the reported CMC and CCC values. This result suggests that chronicand acute effects on aquatic organisms exposed to PFOS and PFOA insurface waters from the six major rivers and lakes in Korea were notlikely.

Furthermore, the reported water concentration of PFOS that is pro-tective of avian wildlife was also determined to be 47 ng L−1 by Giesyet al. (2010). This value was calculated as the geometric mean of threeavian wildlife values for herring gull, bald eagle and kingfisher, whichwere 41 ng PFOS/L, 71 ng PFOS/L and 36 ng PFOS/L, respectively. Inthe present study, the highest concentration of PFOS found in watersamples was less than this avian wildlife protection value. This result

PFUnA PFDoA PFHxS PFOS PFDS ∑PFASsa

0.19–0.32(0.24)

0.10–0.12(0.11)

ND–0.72(0.39)

0.83–1.84(1.27)

ND 2.31–5.71(3.85)

ND ND 0.50–3.97(2.03)

0.67–6.25(3.30)

ND 1.17–10.86(5.90)

0.28–1.13(0.59)

0.13–0.33(0.20)

0.89–1.71(0.21)

6.27–8.46(7.36)

ND 14.71–40.63(26.00)

0.17–0.21(0.20)

0.07–0.13(0.10)

0.23–0.37(0.32)

0.87–1.06(0.98)

ND 7.09–9.61(8.01)

0.10–0.13(0.12)

0.06–0.08(0.06)

0.03–0.11(0.07)

0.25–0.99(0.59)

ND 1.51–1.83(1.70)

0.13–0.73(0.41)

0.10–0.31(0.21)

0.42–1.63(1.03)

1.18–15.07(11.06)

ND 8.47–25.19(18.68)

ND–1.13(0.25)

ND–0.33(0.11)

ND–3.97(0.90)

ND–15.07(3.89)

ND 1.17–40.63(10.44)



Table3

Conc

entration(n

gg−

1dw

)of

PFASs

insedimen

tsho

wed

inmin–max

(mea

n).

Site

(n)

PFHxA

PFHpA

PFOA

PFNA

PFDA

PFUnA

PFDoA

PFHxS

PFOS

PFDS

∑PF

ASs

a

Bukh

an(3)

ND–0.03

(0.02)

ND

ND–0.09

(0.04)

ND–0.05

(0.02)

ND–0.03

(0.01)

ND–0.08

(0.04)

0.02

–0.11

(0.07)

ND–0.01

(0.01)

0.01

–0.07

(0.04)

ND

0.03

–0.40

(0.25)

Nam

han(12)

ND–0.05

(0.01)

ND–0.06

(0.01)

0.03

–0.28

(0.07)

ND–0.12

(0.02)

0.01

–0.08

(0.03)

ND–0.08

(0.04)

0.01

–0.04

(0.03)

ND

0.02

–0.04

8(0.18)

ND

0.12

–1.09

(0.39)

Nak

dong

(3)

ND–0.01

(0.01)

ND

0.04

–0.08

(0.06)

ND–0.03

(0.01)

0.02

–0.07

(0.05)

0.03

–0.08

(0.06)

0.07

–0.08

(0.08)

ND–0.01

(0.00)

0.04

–0.27

(0.16)

ND

0.21

–0.55

(0.43)

Nam

(3)

ND

ND

0.03

–0.09

(0.05)

ND–0.10

(0.06)

ND–0.04

(0.02)

0.04

–0.09

(0.06)

0.06

–0.13

(0.09)

ND–0.01

(0.00)

0.02

–0.12

(0.05)

ND

0.17

–0.57

(0.35)

Sang

sa(3)

ND

ND

0.02

–0.03

(0.03)

ND–0.09

(0.04)

ND–0.04

(0.02)

0.02

–0.03

(0.03)

0.06

–0.09

(0.07)

0.01

–0.01

(0.01)

0.04

–0.04

(0.04)

ND

0.20

–0.25

(0.23)

Yeon

gsan

(3)

ND

ND

ND–0.05

(0.02)

0.09

–0.15

(0.12)

0.03

–0.04

(0.03)

0.02

–0.04

(0.03)

0.06

–0.08

(0.07)

ND–0.01

(0.00)

0.05

–0.11

(0.07)

ND

0.33

–0.36

(0.35)

Allsamplingsites(27)

ND–0.05

(0.01)

ND–0.06

(0.00)

ND–0.28

(0.05)

ND–0.15

(0.04)

ND–0.08

(0.03)

ND–0.09

(0.04)

0.01

–0.13

(0.05)

ND–0.01

(0.00)

0.01

–0.48

(0.12)

ND

0.03

–1.09

(0.35)

n:nu

mbe

rof

analyzed

sample;

ND:b

elow

themetho

dde

tectionlim

it.

a∑

PFASs

referto

sum

oftende

tectab

lePF

ASin

each

samplingsite.


indicates that the concentrations of PFOS inwater samples fromall sam-pling sites in the present study are unlikely to cause potential harmfuleffects to avian wildlife.

3.2. PFASs in sediment

The distribution of PFASs concentration in sediment samples is sum-marized in Table 3. Approximately 2/3 of the sediment samples ana-lyzed in this study contained PFASs above the detection limits. Similarto that inwater samples, PFDSwas not detected in any of sediment sam-ples (Table 1). PFOS and PFDoA were found in all analyzed sedimentsamples. Mean PFOS concentration in sediments was 0.12 ng g−1 dw,which accounted for 32% of the total PFAS concentrations in sediments.Themeasured PFOS concentrations from sediments in the present studywere lower than those reported previously from Koreanwestern coasts(Naile et al., 2010; min = 2 ng g−1 dw), Roter Main River in Germany(Becker et al., 2008; mean = 0.21 ng g−1 dw), Dailao River system inChina (Bao et al., 2009; mean=0.21 ng g−1 dw), Yangtze River estuaryin China (Pan and You, 2010; mean = 536 ng g−1 dw), Tokyo Bay inJapan (Sakurai et al., 2010; mean= 0.54 ng g−1 dw) and San FranciscoBay in the USA (Higgins et al., 2005; mean = 0.85 ng g−1 dw), butwere comparable with those described from Liao River in China(Yang et al., 2011; mean = 0.15 ng g−1 dw), Taihu Lake in China(Yang et al., 2011; mean = 0.15 ng g−1 dw) and Southern Rivers ofJapan (Nakata et al., 2006; range: 0.09–0.14 ng g−1 dw). PFDoA(mean = 0.05 ng g−1 dw) was the next predominant PFAS foundin the sediments. PFDoA levels in sediments were 13 to 48 fold lowerthan those from Uji River (mean = 0.75 ng g−1 dw), Tenjin River(mean = 2.4 ng g−1 dw), or in Kamo River (0.94 ng g−1 dw), andKatsura River (1.7 ng g−1 dw) in Japan (Senthilkumar et al., 2007),but were higher than those from Liao River (mean = 0.01 ng g−1 dw)and Taihu Lake (mean = 0.03 ng g−1 dw) in China (Yang et al., 2011).Following PFDoA, PFOA was found as the next dominant PFAS in thesediments. Detailed comparisons of PFOS and PFOA concentrationfound in the present study with those reported in previous studies areprovided in the Supplementary information.

Similar to PFDoA and PFOA, other long-chain perfluorocarboxylates(LCPFCAs) including PFNA, PFDA and PFUnA were detected in sedi-ments with high detection frequency (Table 1). This result is compara-ble with that in sediment samples from the Liao River and Taihu River,China (Yang et al., 2011). High percentages of mean concentrations ofthese LCPFCAs to total PFASs concentration in sediment samples werefound consistently in all studied rivers and lakes at 71.8%, 50.6%,63.3%, 85.2%, 79.1% and 79.8% in Bukhan River, Namhan River, NakdongRiver, NamRiver, Sangsa Lake and Yeongsan River, respectively. This re-sult suggests that these LCPFCAs are dominant chemicals for sorptionprocess on freshwater sediment samples in the present study.

Partition coefficients of PFASs between sediment and surface water(Kd), which is estimated by the ratio of the concentration of PFASs inthe sediment (ng g−1dw) to the concentration of PFASs in the overlyingwater (ng/L) at the same sampling sites, were used to evaluate PFASs dis-tribution patterns in the sediment samples. Themean Kd values are sum-marized in Table 4. An ascending order of mean Kd for LCPFCAs of PFOA(0.04) b PFNA (0.10) b PFDA (0.13) b PFUnA (0.21) b PFDoA (0.72)was found. The positive association between Kd value with the numberof perfluorocarbon chain length obtained in the present study is consis-tent with that described by Higgins and Luthy (2006). It is worth notingthat Higgins and Luthy (2006) reported that perfluorocarbon chainlength was the dominant structural feature influencing sorption, witheach CF2 moiety contributing 0.50–0.60 log units to the measured fresh-water–sediment distribution coefficients of perfluorinated surfactants.However, PFOS and PFOA had different Kd values. Mean Kd value forPFOS was higher than that for PFOA in most sampling sites. This differ-ence may be caused by the effect of the sulfonate moiety, which contrib-uted an additional 0.23 log units to themeasured distribution coefficient,when compared to carboxylate analogs (Higgins and Luthy, 2006).

Please cite this article as: Lam N-H, et al, Perfluorinated alkyl substances in water, sediment, plankton and fish from Korean rivers and lakes: Anationwide survey, Sci Total Environ (2014), http://dx.doi.org/10.1016/j.scitotenv.2014.01.045


Table 4Mean partition coefficients (Kd) of PFASs between sediment and surface water.

Site (n) PFHxA PFHpA PFOA PFNA PFDA PFUnA PFDoA PFHxS PFOS PFDS

Bukhan (3) 0.09 – 0.06 0.03 0.10 0.18 0.63 0.01 0.04 –

Namhan (2) – 0.12 – 0.15 – – 0.00 0.16 –

Nakdong (3) – – 0.01 0.01 0.05 0.17 0.46 – 0.02 –

Nam (3) – – 0.01 0.10 0.09 0.31 0.98 0.01 0.06 –

Sangsa (3) – – 0.07 0.26 0.29 0.24 1.11 0.13 0.09 –

Yeongsan (3) – – 0.01 0.16 0.09 0.14 0.44 – 0.02 –

All sampling sites (17) 0.02 – 0.04 0.10 0.13 0.21 0.72 0.03 0.07 –

n: number of sampling site.


3.3. PFASs in biota

The concentration profiles of PFASs in plankton samples are shown inTable 5. PFHxA, PFHpA, PFOA, PFHxS, and PFDS were not detected in anyplankton samples. Despite the highest detection frequency of PFNA (83%),the greatest mean PFASs concentration was observed for PFOS (2.08 ngPFOS/gww) in plankton samples. It isworth to note that the next greatestmean PFAS concentration was for PFDoA at 0.36 ng g−1ww, which wasapproximately 6-fold less than the mean concentration of PFOS. Themean concentrations of remaining PFASs were in the order of PFNAN PFUnA N PFDA N PFDoA. Very few studies have measured PFASs inplankton. The mean concentration of PFOS in zooplankton samples ana-lyzed in this study was relatively less than that reported from China (Liet al., 2008; 4.18 ng g−1ww), or from the Barents Sea (Haukås et al.,2007; mean = 3.85 ng g−1ww) but was higher than that reported fromWestern Arctic (Powley et al., 2008; max. = 0.2 ng g−1ww) and EasternArctic (Tomyet al., 2004;mean=1.8 ng g−1ww). PFNAwas not detectedin zooplankton samples from the Barents Sea (Haukås et al., 2007)but was found in a sample from Beijing, China (Li et al., 2008;0.15 ng g−1ww). Although PFOA was not detected in any planktonsamples in the present study and in zooplankton samples from

Table 5Concentration of PFASs in plankton samples (ng g−1ww) showed in min–max (mean).

Sampling media (n) PFNA PFDA PFUnA

Phytoplankton (4) 0.30–0.50 (0.43) ND–0.39 (0.10) ND–0.2Micro-zooplankton (4) ND–0.40 (0.20) ND ND–0.4Meso-zooplankton (4) ND–0.50 (0.25) ND ND–0.2

n: number of analyzed sample; ND: below the method detection limit.a ∑PFASs refer to sum of ten detectable PFAS in each sampling site.

Table 6Range and mean concentration (ng g−1ww or ng mL−1) of PFASs in fish tissues.

Crucian carp (n = 69)

f/m (n.d.)* 50/18 (1)BW (g) 76.40 ∼ 973.19 (237.74)BL (cm) 12.50 ∼ 32.00 (19.40)HSI 0.45 ∼ 7.71 (2.93)GSI 0.29 ∼ 16.23 (5.05)

Concentration Blood Liver

PFHxA ND ∼ 0.36 (0.02) NDPFHpA ND NDPFOA ND ∼ 0.89 (0.09) ND ∼ 0.33 (0.03)PFNA ND ∼ 13.22 (1.46) ND ∼ 0.86 (0.07)PFDA 0.44 ∼ 20.58 (5.15) 0.06 ∼ 3.48 (0.75PFUnA 0.88 ∼ 45.16 (7.11) 0.04 ∼ 5.01 (0.80PFDoA 0.11 ∼ 19.18 (3.20) ND ∼ 2.08 (0.43)PFHxS ND ∼ 4.96 (0.17) ND ∼ 0.30 (0.01)PFOS 0.18 ∼ 145.23 (13.93) ND ∼ 43.76 (6.15PFDS ND ∼ 0.60 (0.04) ND ∼ 0.58 (0.05)∑PFASs** 1.72 ∼ 236.29 (31.18) 0.15 ∼ 54.64 (8.2

BW: body weight; BL: body length; ND: below the method detection limit; n: number of analyaf/m (n.d.): female/male (not determined).b∑PFASs refer to sum of ten detectable PFAS in each individual fish.


Bank Island, Western Arctic (Powley et al., 2008), this chemicalwas found at relatively high concentration in zooplankton collectedfrom Frobisher Bay (Tomy et al., 2004; mean = 2.6 ng g−1ww), Ba-rents Sea (Haukås et al., 2007; mean = 3.15 ng g−1ww) andGaobeidian Lake (Li et al., 2008; mean = 0.05 ng g−1ww).

Concentrations of PFASs in blood and liver of crucian carp and man-darin fish are summarized in Table 6. PFHpA was not detected in all in-vestigated fish tissues. PFOS was consistently found at the highestconcentration and accounted for 37%, 57%, 49% and 52% of the totalPFASs concentration in crucian carp blood, crucian carp liver, mandarinfish blood and mandarin fish liver, respectively. Following PFOS, PFUnAwas the next predominant PFAS in fish tissues. PFOS and PFUnA werealso reported as the predominant PFASs found in both liver samplesfrom marine mammals from Korean coastal waters (Moon et al.,2010) and skipjack tuna collected from offshore waters and someopen ocean sites in the Sea of Japan, the East China Sea, the IndianOcean, and the Western North Pacific Ocean (Hart et al., 2008). In thepresent study, PFUnA was found in all fish tissues samples. The detect-ing frequency of PFOS and PFDoAwas 100% in crucian carp andmanda-rin fish blood samples and the detecting frequency of PFDAwas 100% incrucian carp blood and liver samples. The sum concentrations of these 4

PFDoA PFOS ∑PFASsa

7 (0.13) ND–0.71 (0.26) ND–0.70 (0.21) 0.30–2.15 (1.12)4 (0.17) ND–0.96 (0.43) ND–11.07 (2.82) 0.10–12.47 (3.61)7 (0.10) ND–1.08 (0.39) ND–12.67 (3.21) 0.20–12.98 (3.94)

Mandarin fish (n = 20)

12/7 (1)52.58 ∼ 424.60 (134.85)15.20 ∼ 29.40 (19.27)0.79 ∼ 3.01 (1.67)0.09 ∼ 2.77 (0.63)

Blood Liver

ND NDND ND0.06 ∼ 0.34 (0.19) 0.09 ∼ 0.33 (0.13)0.03 ∼ 1.00 (0.21) ND

) ND ∼ 28.33 (12.20) 0.38 ∼ 5.78 (1.68)) 9.98 ∼ 52.39 (20.32) 1.93 ∼ 8.04 (4.53)

3.10 ∼ 13.94 (6.74) 0.92 ∼ 3.17 (1.76)ND ND

) 3.68 ∼ 233.68 (60.62) 1.61 ∼ 114.99 (19.38)0.08 ∼ 1.27 (0.44) ND ∼ 0.23 (0.01)

9) 31.08 ∼ 296.72 (100.72) 6.13 ∼ 131.58 (6.13)

zed sample.



0

20

40

60

PFOS

0

1

2

3

4

0 100 200 0 20 40

PFDA

Liv

er c

once

ntra

tion

(ng/

g w

w)

Blood concentration (ng/ml)

Fig. 4. Relationship between PFOS, PFDA concentrations in blood and those in liver incrucian carp (Spearman's correlation, n = 69, rPFOS = 0.953, pPFOS b 0.001; rPFDA =0.494, pPFDA b 0.001).

100 PFOS6

PFDA

ww

)


dominant PFASs including PFOS, PFUnA, PFDoA and PFDA accounted for94–99% of the total PFASs concentration in fish (Fig. 3).

The concentrations of PFOS in fish blood ranged from 0.18 to145 ng mL−1 (mean = 13.9 ng mL−1) in crucian carp and from 3.68to 234 ng mL−1 (mean = 60.6 ng mL−1) in mandarin fish. The next 3abundant PFASs were in the order of, PFUnA (mean = 7.11 ng mL−1)N PFDA (mean = 5.13 ng mL−1) N PFDoA (mean = 3.2 ng mL−1) incrucian carp blood and at mean concentration of 20.3 ng mL−1

N 12.2 ngmL−1 N 6.74 ngmL−1 inmandarin fish blood.Mean PFOS con-centrations in fish blood analyzed in this study were relatively lowerthan those reported for blood of mullet from Shihwa Lake, Korea (Yooet al., 2009); crucian carp and common carp from Gaobeidian Lake,China (Li et al., 2008); a variety of fish collected from Tokyo Bay,Osaka Bay, Biwa Lake in Japan (Taniyasu et al., 2003); dolphin andbluefin tuna from Italian coast (Kannan et al., 2002b) but higher thanthose in the blood of shad from Shihwa Lake, Korea (Yoo et al., 2009);and white semiknife carp, tilapia and leather catfish in China (Li et al.,2008).

The profiles of PFOS concentration in fish liver varied widely. Themaximum concentration of PFOS in fish liver was 115 ng g−1ww in amandarin fish liver sample. The mean concentration of PFOS in fishliver samples and other aquatic animals collected from Korea (Moonet al., 2010), Japan (Taniyasu et al., 2003) or the USA (Sinclair et al.,2006) was relatively higher than that found in the present study. PFOSconcentrations from skipjack tuna in the oceans (Hart et al., 2008) andPFDA, PFUnA and PFDoA concentrations in fish liver from Korea (Yooet al., 2009) were higher than those reported for crucian carp butlower than those reported for mandarin fish in the present study.PFNA concentration found in fish liver tissues in the present study waslower than that reported for rockfish, shad and mullet from Korea(Yoo et al., 2009). More detail comparisons of PFOS and PFOA concen-trations obtained in biota sample from the present study with those re-ported in previous studies are provided in the Supplementaryinformation.

Significant positive correlations (p b 0.001) between PFAS concen-trations in blood and corresponding concentrations in liver werefound for PFOS and PFDA in both crucian carp and mandarin fish(Figs. 4 and 5). Additionally, Spearman's correlation analysis showedthe significant positive correlation between concentrations amongPFOA, PFNA, PFDA, PFUnA, PFDoA, PFDS (p b 0.01) and PFHxS (pb 0.05) in crucian carp blood and liver. However, strong significant cor-relations (p b 0.01 and r N 0.8) between PFASs concentration in fishblood and liver were only observed for PFOS, PFUnA, PFDoA in cruciancarp and PFOS in mandarin fish. These results suggest that blood canbe used for nonlethal monitoring of PFASs in fishes.

The ratio of PFAS concentrations in fish blood to corresponding con-centrations in fish liver variedwidely. The ratio of PFOS concentration inblood to liver varied from 0.71 to 5.17 (mean = 2.31) in crucian carpand from 0.75 to 12.5 (mean = 4.81) in mandarin fish. These observa-tions suggest a non-equilibrium in PFAS concentrations between liverand blood of fish, and indicate an ongoing exposure of fish to PFASs

0% 20% 40% 60% 80% 100%

Carp blood

Carp liver

Mandarin blood

Mandarin liver

PFOS PFDA PFUnA PFDoA PFNAPFHxA PFHpA PFOA PFHxS PFDS

Fig. 3. Patterns showing relative concentrations of individual PFASs (mean-%-composi-tion) in the surveyed fish tissues. PFOS, PFUnA, PFDA and PFDoA were 4 predominantPFASs in the fish tissues and accounted averagely for 97.47% of total PFASs concentration.


(Taniyasu et al., 2003). Furthermore, physiological conditions (e.g., re-productive stages) may play a role in the alteration of blood to liver ra-tios in concentrations of PFASs (Kannan, 2011).

A significant negative correlation was observed between HSI andblood to liver ratio of PFOS and PFNA (p b 0.05) in crucian carp. Theblood to liver concentration ratio of PFOS and PFNA, thus, decreasedwith increasing HSI in crucian carp. A significant positive correlationwas found between GSI and blood to liver ratio of PFOS (p b 0.05) inmandarin fish. The blood to liver ratio of PFOS, therefore, increasedwith increasing sexual maturity of mandarin fish, which is representedby GSI.

Some previous studies have reported gender-specific differences inthe PFAS concentrations in aquatic animals (Keller et al., 2005;Kannan et al., 2002b). In the present study, there was no significant dif-ference (p N 0.05) in all PFAS concentrations between sexes of fish tis-sues except for PFNA in mandarin fish blood. The PFNA concentrationin female mandarin fishes was significantly greater than that in males(p b 0.05).

PFNA was also the only PFAS that has the significant positive corre-lation with crucian carp body weight and body length (p b 0.05).These results suggest different PFAS composition profiles in the sur-veyed fish and chemical compound-specific, fish species-specific andtissue-specific bioaccumulation of PFASs.

3.4. Bioconcentration factor (BCF)

MeanBCFs of PFASs in biota are shown in Table 7. An increasing levelof mean concentrations of PFOS was found in biota with the increase in

0

25

50

75

0

2

4

0 100 200 300 0 20 40

Liv

er c

once

ntra

tion

(ng/

g

Blood concentration (ng/ml)

Fig. 5.Relationship between PFOS, PFDA concentrations in blood and those in liver inman-darin fish (Spearman's correlation, n = 20, rPFOS = 0.880, pPFOS b 0.001; rPFDA = 0.675,pPFDA = 0.001).



Table 7Mean bioconcentration factor of PFASs (L/kg) in biota.

PFASs Phyto-plankton Microzoo-plankton Mesozoo-plankton Carp liver Carp blood Mandarin liver Mandarin blood

PFHxA – – – – 125 – –

PFHpA – – – – – – –

PFOA – – – 134 611 601 739PFNA 1449 – 1562 150 4686 – 855PFDA – – – 5957 34,896 7238 89,216PFUnA – – – 1877 17,328 – –

PFDoA – – – 1945 11,988 – –

PFHxS – – – 8 342 – –

PFOS 196 3017 3450 4572 11,167 24,718 73,612PFDS – – – – – – –


trophic level in the food chain. The BCF of PFOS (concentration in biota/concentration in water) was as follows: phytoplankton (196 L/kg)b zooplankton (3233 L/kg) b crucian carp liver (4567 L/kg) b cruciancarp blood (11,167 L/kg) b mandarin liver (24,718 L/kg) b mandarinblood (73,612 L/kg). This result was consistent with that reported inearlier studies which reported the positive correlations of PFOS concen-trations in biota with the increase in trophic level in the food chain(Giesy and Kannan, 2001; Martin et al., 2004; Tomy et al., 2004; Liet al., 2008).

Mean BCFs of all investigated PFASs in fish blood were higher thanthose in fish liver. The average BCF of PFOS in fish tissues in this studywas relatively higher than those reported in a variety of fishes andsome other aquatic animals in both field and laboratory studies (3M,2003; Moody et al., 2002; Morikawa et al., 2006). Although PFOS con-centrations in water samples were comparable with PFOA concentra-tions, the BCFs of PFOA in biota were 18–100 fold less than those ofPFOS. Apart from PFOS, only PFNA was concentrated in plankton sam-ples. The BCFs of PFNA in phytoplankton and zooplankton were 1449(L/kg) and 1312 (L/kg), respectively.

4. Conclusions

The results of this study indicate a general ascending order of PFASconcentration in freshwater aquatic ecosystem comprising water, sedi-ment, plankton, crucian carp tissues, and mandarin fish tissues. PFOSwas consistently detected at the greatest concentrations throughoutthe investigated media. No potential chronic and/or acute effects onaquatic organismsdue to PFOS and PFOA levelsmeasured in surfacewa-ters from the six major rivers and lakes were expected.

The rank order of mean BCF of PFOS in biota was; phytoplanktonb zooplankton b crucian carp liver b crucian carp blood b mandarinfish liver b mandarin fish blood. The data from the present study alsodemonstrate that PFOS and LCPFCAs have high BCFs in crucian carp tis-sues; only PFOS and PFNA were concentrated in plankton samples. Dif-ferent PFAS composition patterns in fish tissues suggest species-specificand tissue-specific bioaccumulation.

The profiles of occurrence and spatial distribution of PFASs in variousenvironmental media suggest the existence of several sources of PFASsand the continuing input PFASs in Korean rivers and lakes. WWTP dis-charges are a source of PFASs in freshwater ecosystems in SouthKorea. Further study should focus on identifying the existence and sta-tus of PFASs sources in South Korean freshwater ecosystems.

Conflict of interest

The authors declare no conflict of interest.

Acknowledgments

This study was funded by the National Institute of EnvironmentalResearch (NIER) of Korea (NIER/2010/1697 grant and NIER/SP2012/166 grant).


Appendix A. Supplementary data

Supplementary data to this article can be found online at http://dx.doi.org/10.1016/j.scitotenv.2014.01.045.

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