Elsevier

Chemosphere

Volume 176, June 2017, Pages 165-174
Chemosphere

Long-term trends in dietary intake of perfluoroalkyl carboxylic acids in relation to their serum concentration in two regions in Japan from 1979 to 2011

https://doi.org/10.1016/j.chemosphere.2017.02.073Get rights and content

Highlights

  • Perfluoroalkyl carboxylic acids (PFCAs) in diet and serum have been investigated.

  • The analyzed samples obtained since the 1980s until the 2010s.

  • A positive correlation was observed between diet and serum concentration of PFCAs.

  • This indicates that dietary intake may be a source of C8–C11 PFCAs exposure.

Abstract

We investigated temporal changes of perfluoroalkyl carboxylic acids (PFCAs) with 8–14 carbon atoms (C8 to C14) in duplicate diet and serum samples in Japan. The sum dietary intakes of PFCAs (C8 to C13) in the Kansai and Tohoku region were highest in the 2010s (mean; 177 ng/day for Kansai, 107 ng/day for Tohoku) followed by the 2000s (77 ng/day for Kansai, 34 ng/day for Tohoku) and the 1990s (53 ng/day for Kansai, 58 ng/day for Tohoku), then the 1980s (19 ng/day for Kansai, 23 ng/day for Tohoku). The sum of the serum concentartions (C8 to C13) was also highest in the 2010s (mean; 17 ng/mL for Kansai, 7.4 ng/mL for Tohoku), followed by the 2000s (12 ng/mL for Kansai, 6.3 ng/mL for Tohoku), then the 1990s (6.8 ng/mL for Kansai, 5.5 mg/mL for Tohoku) and the 1980s (3.8 ng/mL for Kansai, 0.4 ng/mL for Tohoku). A positive correlation was observed between dietary intakes and serum concentration for C8 to C11 (r = 0.94, p < 0.05 for C8; r = 0.80, p < 0.05 for C9; r = 0.98, p < 0.05 for C10; and r = 0.84, p < 0.05 for C11). The levels of C8, C9 and C10 in serum and dietary intake in the 2010s were much higher in Kansai than those in Tohoku, although those of C11 did not show such differences. Kansai has a fluoropolymer manufacture known as a specific source of PFOA (C8), and is more urbanized than Tohoku, which may be attributed to the higher levels of PFCAs (C8 to C10). On the other hand, C11 is common to residents in Kansai and Tohoku.

Introduction

Perfluoroalkyl carboxylic acids (PFCAs) are carboxylic acids with a perfluoroalkyl chain, where all the hydrogen atoms have been replaced by fluorine atoms (Kissa, 2001). PFCAs persist in the environment, as they cannot decompose in the ecosystem (ECHA). The PFCA with eight carbon atoms is called perfluorooctanoic acid (PFOA or C8), and has been used for the manufacture of fluoropolymer resin (Scheirs, 1997).

Previous animal studies have revealed the potential toxicities of PFCAs, particularly developmental toxicity (Case et al., 2001), immune toxicity (Yang et al., 2002), and hepato-toxicity (Klaunig et al., 2003, Lau et al., 2007). Recently, a systematic review concluded that there was sufficient evidence that developmental exposure to PFOA reduces fetal growth in humans (Johnson et al., 2014). Epidemiological studies demonstrated that PFCAs can suppress antibody production after immunization against tetanus and diphtheria in children (Grandjean et al., 2012), and have been linked to miscarriage (Jensen et al., 2015). PFCAs therefore have potential health risks in the general population.

Major fluoropolymer manufacturers have pledged to try to reduce PFOA emissions under a stewardship program by the US Environmental protection agency (EPA, 2015). In Japan, Daikin Industry in Osaka, Kansai region, announced that PFOA emissions in 2012 were less than 1% of that in 2000 (Daikin, 2012). To evaluate the effect of those voluntary reductions, follow-up monitoring for PFOA and other PFCAs in diet and serum over long periods of time is needed.

Several previous studies around the world have reported temporal PFCA trends in human serum from around 1995 to the 2010s (Calafat et al., 2007, Harada et al., 2011, Kato et al., 2011, Glynn et al., 2012, Gebbink et al., 2015b). According to these reports, long-chain PFCAs (>C8) levels in human serum have been increasing since around the 2000s, although PFOA levels have decreased since 2002 (Calafat et al., 2007, Harada et al., 2011, Glynn et al., 2012). More recently, long-term PFCA trends (1982–2009) in human serum were evaluated in Germany (Yeung et al., 2013), and the C9 compound showed a transient elevation from 1982 to 1990, which was not observed in the other countries.

Previous reports have also described PFCA levels in food samples (D'Hollander et al., 2010, Haug et al., 2010, Noorlander et al., 2011, Vestergren et al., 2012, Klenow et al., 2013, D'Hollander et al., 2015). For PFOA, exposure modeling studies have shown that dietary exposure is the major exposure pathway in most of general population (Trudel et al., 2008, Fromme et al., 2009, Vestergren and Cousins, 2009, Niisoe et al., 2010). However, the importance of different exposure pathways of PFCAs longer than PFOA (C8) for humans is still ambiguous (D'Eon et al., 2011, Gebbink et al., 2015a).

In the present study, we evaluated the concentration of PFCAs (C8 to C14) in diet composite samples from 1979 to 2011 in two different regions in Japan. We used duplicate sampling methods; all food and drink items include tap water for drinking that was consumed over a 24-h period. This method evaluates the dietary exposures which are very close to actual levels. We also analyzed serum samples, which were collected at corresponding time points and regions. Ecological evaluation of both diet duplicate and serum samples over three decades allowed us to assess whether long-term trends of serum PFCA concentrations is associated with dietary PFCA intakes.

Section snippets

Sample collection

We used archived samples from the Kyoto University Human Specimen Bank (Koizumi et al., 2005, Koizumi et al., 2009). Details of the target population and sampling regions are shown in Table S1 and Fig. S1. Kansai is located in the central of the main island of Japan, while Tohoku is in the north of the same island. The Kansai region is more urban than the Tohoku region. The Kansai region had around 20 million residents in 2014, while the Tohoku region had 9 million residents (MIC, 2016).

Temporal trends of dietary PFCAs intake

Dietary intakes of PFCAs (ng/day) are presented in Table 1. The percentage samples with detectable PFCAs ranged from 57% to 86% in aggregate average for all diet samples for C8 to C13 (86% for C8, 82% for C9, 66% for C10, 81% for C11, 57% for C12, and 65% for C13) and only 7% for C14. In the Kansai region, the total intake of the C8 to C13 PFCAs (ΣC8 to C13, mean) was lowest in the 1980s (19 ng/day in 1979), followed by the 1990s (53 ng/day in 1993), the 2000s (77 ng/day in 2003/2004), and then

Conclusion

In the present study, we have described the long-term PFCAs trends in two regions in Japan. Our study revealed that from the 1980s to the 2010s, serum levels of C11 and C13 exhibited a large and rapid increase between the 1980s and the 1990s in sharp contrast to those in Europe, and exhibited a slow increase or slight decrease from the 1990s to the 2010s. The serum levels of C8, C9 and C10 PFCAs were higher in Kansai, while those of C11 and C13 were the same level across both Kansai and Tohoku

Acknowledgments

This study was supported by the Special Coordination Funds for Promoting Science and Technology (Grant No. 1300001) sponsored by the Japan Science and Technology Agency, a Grant-in-Aid for Health Sciences Research from the Ministry of Health, Labour and Welfare, Japan (Grant Nos. H21-Food-003 and H24-Food-002) and JSPS KAKENHI Grant Numbers 16K00565 and 26881008. The funding bodies had no role in the study design, data collection, or analysis, or in decisions concerning the preparation and

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