Elsevier

Journal of Hazardous Materials

Volume 279, 30 August 2014, Pages 402-409
Journal of Hazardous Materials

Foodstuff analyses show that seafood and water are major perfluoroalkyl acids (PFAAs) sources to humans in Korea

https://doi.org/10.1016/j.jhazmat.2014.07.004Get rights and content

Highlights

  • 16 PFAAs in 397 samples of 66 food types and 34 tap water samples were analyzed.

  • Dietary exposure to PFAAs was estimated by using the PFAAs measured concentrations.

  • The major contributors of PFAAs dietary exposure were confirmed.

Abstract

We measured concentrations of PFAAs in 397 foods, of 66 types, in Korea, and determined the daily human dietary PFAAs intake and the contribution of each foodstuff to that intake. The PFAAs concentration in the 66 different food types ranged from below the detection limit to 48.3 ng/g. Perfluorooctane sulfonate (PFOS) and long-chain perfluorocarboxylic acids (PFCAs) were the dominant PFAAs in fish, shellfish, and processed foods, while perfluorooctanoic acid (PFOA) and short-chain PFCAs dominated dairy foodstuffs and beverages. The Korean adult dietary intake ranges, estimated for a range of scenarios, were 0.60–3.03 and 0.17–1.68 ng kg−1 bw d−1 for PFOS and PFOA, respectively, which were lower than the total daily intake limits suggested by European Food Safety Authority (PFOS: 150 ng kg−1 bw d−1; PFOA: 1500 ng kg−1 bw d−1). The major contributors to PFAAs dietary exposure varied with subject age and PFAAs. For example, fish was a major contributor of PFOS but dairy foods were major contributors of PFOA. However, tap water was a major contributor to PFOA intake when it was the main source of drinking water (rather than bottled water).

Introduction

Perfluoroalkyl and polyfluoroalkyl substances (PFASs) including PFAAs, fluorotelomer alcohols (FTOHs), and etc. have been widely used in industry as surfactants, polymer and plastic additives, and, etc. because of their oleophobic and hydrophobic characteristics [1], [2], and they have been found to be ubiquitous in the environment, including in humans and foods [3], [4]. Especially, PFOS and its salts were added to Annex B of the Stockholm Convention on Persistent Organic Pollutants (POPs) in 2009, and now regarded as emerging POPs. Toxicological studies of PFASs in animals have shown that they are hepatotoxic, cause developmental and reproductive disturbances, and that they may have adverse health effects on humans [5], [6], [7], [8]. PFASs are also known to easily accumulate in humans by combining with proteins [2], [6], [9]. Several sources of and pathways for human exposure to PFASs have been suggested [10], [11], [12], [13], [14]. Diet (particularly fish intake) is widely accepted as being a major source of PFASs to humans, because of previous food analysis studies [15], [16], [17] and correlations between PFASs concentration in human serum and dietary habit data from surveys [18], [19], [20]. Human dietary intakes of PFASs have been estimated in several countries [10], [14], [21], [22]. For example, the median dietary intakes of PFOS and PFOA, calculated from the analysis of 214 duplicate diet samples, were 1.4 and 2.9 ng kg−1 bw d−1, respectively, in Germany [23]. Mean dietary intakes of 18 ng d−1 for PFOS and 31 ng d−1 for PFOA were calculated from the results of the analysis of 21 food samples from Norway [14]. Dietary intakes of PFOS have been estimated to be 100–250 ng d−1 in the UK [21], USA [24], and Canada [10]. The differences in estimated daily intakes (EDIs) from different studies and countries might be caused by different foods and different numbers of samples being analyzed, different detection limits and target PFASs, and different food consumption habits in different areas. Recently, several researches including inter-laboratory study on PFASs in food samples, made an effort to improve the analytical methods in dietary samples and found the possibility of errors that could be involved in analytical processes [15], [25], [26]. There have only been a small number of comprehensive studies in which the diverse range of major foods that the general population in a country consume have been analyzed, even though it is necessary to analyze a wide range of foods to accurately estimate dietary exposure to PFASs. Of many studies in which EDIs have been calculated, EDIs have only been estimated from national total diet studies in Canada and the Netherlands [10], [15], [27], most other studies having been based on data from a small number of samples and a limited selection of food [14], [28], [29]. Diverse ranges of contributors to human exposure to PFASs have been investigated in many studies. Meat has been suggested to be the primary contributor to dietary exposure to PFOA [30]. Fish consumption was major dietary contributor of long-chain PFAAs [31] and drinking water, has been proposed to be major contributors to exposure to PFASs in general [32]. The differences in the major contributors to human dietary exposure to PFASs that have been suggested show that it is necessary for more dietary intake studies to be performed, with large numbers of samples and food types being analyzed, to ensure that such studies are representative of the total dietary intake of the general population.

In the study, 16 PFAAs in 397 samples of 66 food types from South Korea were analyzed to assess the PFAAs contamination in different types of food and to determine the main contributors to human exposure to PFAAs. We used the monitoring results to calculate the daily dietary intake of PFAAs. To the best of our knowledge, this is the first study of PFAAs concentrations in a wide range of foodstuffs and of human dietary intakes of PFAAs in Korea, and we believe that this is one of the most comprehensive monitoring studies of PFAAs in foodstuffs that has been performed worldwide.

Section snippets

Sample collection

A total of 397 food samples were collected from a market in Busan, which is the second largest city in Korea, in 2011 (n = 227) and 2012 (n = 170). The food samples were of 66 different food types, and were classified into seven food categories, which were fish and shellfish, meat and meat products, vegetables and fruits, processed products, dairy products, beverages, and others. The foodstuffs selected accounted for 90% of the typical daily diet for the Korean population [33]. Processed and

PFAAs concentrations in a wide range of food samples

The concentrations of the 16 PFAAs and the frequencies at which they were detected in the 66 different domestic food types that were analyzed are presented in Table 1. PFAAs concentrations below the LODs were treated as zero when calculating the mean and total (Σ) PFAAs concentrations. As shown in Fig. 1, fish and shellfish contained the highest mean ΣPFAAs concentration (2.34 ng/g), followed by meat and meat products (1.61 ng/g), processed products (0.85 ng/g), dairy products (0.57 ng/g), and then

Acknowledgments

This study was supported by grant 12162KFDA735 from the Korea Food & Drug Administration in 2012 and the Korean Ministry of Environment (MOE) through “The Environment Health Action Program”.

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