Dietary Exposure Estimates for the Food Preservatives Benzoic Acid

Jan 29, 2015 - The purpose was to assess the health risk to general consumers in Taiwan associated with dietary intake of benzoic acid and sorbic acid...
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Dietary exposure estimates for the food preservatives benzoic acid and sorbic acid in the total diet of Taiwan Min-Pei Ling, Keng-Wen Lien, Chiu-Hua Wu, Shih-Pei Ni, Hui-Ying Huang, and Dennis P. H. Hsieh J. Agric. Food Chem., Just Accepted Manuscript • DOI: 10.1021/jf503987y • Publication Date (Web): 29 Jan 2015 Downloaded from http://pubs.acs.org on February 2, 2015

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Journal of Agricultural and Food Chemistry

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Journal of Agricultural and Food Chemistry

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Dietary exposure estimates for the food preservatives benzoic acid and sorbic acid in the total

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diet in Taiwan

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Min-Pei Ling,*,† Keng-Wen Lien,‡ Chiu-Hua Wu,† Shih-Pei Ni,† Hui-Ying Huang,§ Dennis P. H.

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Hsieh†

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Department of Health Risk Management, China Medical University, 91 Hsueh-Shih Road, Taichung, 40402 Taiwan, R.O.C

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Institute of Food Science and Technology, National Taiwan University,1 Sec. 4, Roosevelt Road, Taipei, 10617 Taiwan, R.O.C

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Department of Nutrition, China Medical University, No.91 Hsueh-Shih Road, Taichung, 40402 Taiwan, R.O.C

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* To whom correspondence should be addressed.

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Dr. Min-Pei Ling; Department of Health Risk Management, China Medical University, 91

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Hsueh-Shih Road, Taichung 40402, Taiwan, R.O.C.

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Telephone: +886-4-2205-3366#6508; Fax: +886-4-2207-0429; E-mail:

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[email protected]

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ABSTRACT

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The purpose was to assess the health risk to general consumers in Taiwan associated with

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dietary intake of benzoic acid and sorbic acid by conducting a total diet study (TDS). The hazard

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index (HI) in percent acceptable daily intake (%ADI) of benzoic acid and sorbic acid for eight

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exposure groups classified by age were calculated. In high-intake consumers, the highest HI of

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benzoic acid was 54.1 %ADI for males aged 1-2 years old at the 95th percentile, whereas for

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females, the HI was 61.7 %ADI for aged over 66 years old. The highest HI of sorbic acid for male

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and female consumers aged 3-6 years old at the 95th percentile were 14.0 %ADI and 12.2 %ADI,

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respectively. These results indicate that the use of benzoic acid and sorbic acid as preservatives at

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the current level of use in the Taiwanese diet does not constitute a public health and safety concern.

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KEYWORDS: TDS; food preservatives; risk assessment; benzoic acid; sorbic acid

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INTRODUCTION

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In 1961, U.S. Food and Drug Administration (US FDA) program to monitor radioactive

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contamination in foods, the total diet study (TDS) has been used to measure the dietary intake of

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specific analytes by population groups in countries or defined regions,1 and to assess its associated

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health risk. TDS, also known as a “market basket study”, has been used as a national monitoring

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research tool for food contamination and dietary exposure.2,3 It is based on a national representative

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of food consumption for different subgroups of the general population. TDS can be used to

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determine the levels of various contaminants and nutrients present in foods and to estimate the

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public health risk due to chronic exposure to the presence of chemical substances.4 TDS

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representative foods are designed to measure the average intake of chemicals found in cooked or

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processed foods. In TDS, food samples are prepared prior to analysis as they would be consumed

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(table-ready), so that the analytical results provide the basis for realistic estimation of the dietary

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intake of these analytes and provide a reasonable assessment of the health risk. So far,

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approximately 33 countries in the world have carried out TDS or TDS-like studies, including

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Australia, New Zealand, Canada, People’s Republic of China (Macau and Hong Kong), France,

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Taiwan, Netherlands, United Kingdom and United States of America.5 The classes of food

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chemicals that have been studied in previous TDSs mentioned in the literature include

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radionuclides,6 persistent organic pollutants,7 metals,8 mycotoxins,9 pesticides,10 nutrient

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elements,11 and food additives.12-16 On the other hand, the World Health Organization (WHO)

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indicates that the level of food safety in a country can be adequately understood by a TDS.17 In the

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TDS program, the food contaminant is analyzed after the foods are cooked and table-ready.

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Taiwanese cooking consists of a number of complicated steps and methods; hence TDS provides a

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better estimation of risk from food additives.

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Benzoic acid (C6H5COOH) is naturally present in fruits such as peach, plum, strawberry, apple,

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and cinnamon. It is commonly used as an antiseptic, antimycotic, and antipyretic preservative in

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foods and beverages.18 The use of benzoic acid in several food groups is authorized in the European 3

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Union on the condition that the maximum use rules are respected.19 Directive 95/2/EC also requires

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member states to monitor the consumption and use of food additives in order to allow evaluation of

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consumption trends as well as differences in consumption patterns among various member states.

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Sorbic acid (CH3-CH=CH-CH=CH-COOH) is a short-chain fatty acid with two unsaturated

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bonds. It is widely used in the food, beverage, cosmetic, and other industries. As Taiwan is a

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subtropical country with warm and humid weather, preservatives are widely used to inhibit the

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growth of bacteria, yeasts, and molds to extend the shelf life of food and reduce the possibility of

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food poisoning. Common antimicrobial preservatives include sorbic acid and its salts, benzoic acid

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and its salts, calcium propionate, and sodium nitrite. The excessive use of preservatives may be

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harmful to the body; therefore, it is necessary to control their use in the preparation and preservation

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of food. There are 21 kinds of preservatives that can be used legally in specific food items in

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Taiwan. Benzoic acid, sorbic acid, benzoates, and sorbates are permitted for use as preservatives for

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34 food items. For example, benzoic acid and sorbic acid can be used in soya sauce, tomato sauce,

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and chili sauce to a maximum concentration of 1 g/kg. As Taiwan is quite advanced in food

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manufacturing industry, the use of food additives is rather widespread. Except preservatives, like

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pigments, emulsifiers, and sweeteners a total of 18 types of food additives are permitted for use in

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specific foods, and the additives are prepared by extraction from natural sources or chemical

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synthesis. And the application and the amount of preservatives are regulated by Taiwan Food and

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Drug Administration (TFDA) “Standards for Specification, Scope, Application and Limitation of

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Food Additives List”.20 Items not included in the list are technically not permitted for use in

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processed foods.

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In previous years, TFDA surveys of commercially available foods have found that illegal use

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of preservatives and addition of bleaching agents as food additives are very common in Taiwan.21 It

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was also found that food additives and preservatives are added in amounts that exceed permissible

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limits for their use. Since the majority of the samples in the surveys of marketed foods by local

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government contained benzoic acid and sorbic acid, it is thus important to take a closer look at these 4

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two preservatives due to their popular use. These issues not only pose a risk to public health, but

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also endanger the trade economy. Because of the growing concern regarding levels of preservatives

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in processed food exceeding their acceptable daily intake (ADI), preservative concentrations and

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estimated exposure of the population were subject to investigative examination. A survey of benzoic

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acid in foods in Finland identified fruit, berry juices, soft drinks, and semi-preserved fish as the

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major sources of benzoic acid intake (40 mg/day, 13% of ADI).22 And the 21st Australian TDS also

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estimated the dietary exposure to preservative: benzoates and sorbates. 13

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The specific aims of this study include the following.

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(1) To determine the concentrations of benzoic acid and sorbic acid in foods as consumed,

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(2) To assess exposure and risk with regard to population groups of various ages,

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(3) To identify which food pose the greatest exposure risk to consumers,

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(4) To propose appropriate risk management options to protect consumers.

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This study was deemed necessary, as dietary composition and intake patterns are distinctly different

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from Western countries where similar studies had been reported.

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MATERIAL AND METHOD

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Hazard identification of benzoic acid. Repeated or prolonged exposure to benzoic acid can

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cause chronic health effects and damage to organs. Reproductive toxicity was observed in rats fed

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with benzoic acid at concentrations of 0.5 g/kg of body weight (BW)/day.23 The use of benzoic acid

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with artificial food colors has also been linked to hyperactivity in children.24 The Joint FAO/WHO

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Expert Committee on Food Additives (JECFA) has established an ADI of 0-5 mg/kg of BW/day for

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benzoic acid and benzoates. The no observed effect level (NOEL) was established at the highest

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experimental dose (500 mg/kg of BW/day) at which no adverse effects were observed based on

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long-term (lifetime) studies in rats. In establishing the ADI, a safety factor (SF) of 100 was applied 5

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to the NOEL to take into account species differences and individual human variation25, 26.

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Hazard identification of sorbic acid. Sorbic acid and potassium sorbate were practically

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nontoxic to rats and mice in acute oral toxicity studies.27 They had a very low level of mammalian

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toxicity, even in chronic doses of up to 10% of the diet. They were found to be non-carcinogenic

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and non-mutagenic in vitro and in vivo.28, 29 However, oral toxicity studies showed that intake of

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sorbic acid may result in liver weight gain in 90 days.30 The JECFA has established an ADI of 0-25

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mg/kg of BW/day for sorbic acid and sorbates. The NOEL was established at the highest

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experimental dose (2500 mg/kg of BW/day) at which no adverse effects were observed based on

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long-term (lifetime) studies in rats.31 In establishing the ADI, a SF of 100 was applied to the dose

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level to take into account species differences and individual human variation.32

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Core food list for the Taiwan TDS. A large amount of food consumption data from the

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2005-2008 Nutrition and Health Survey in Taiwan (NAHSIT) are available.33 The sample

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population consisted of 6,104 participants randomly selected from 48 counties. Information on

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dietary intake was collected by two non-consecutive 24 h recalls in combination with a food

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frequency questionnaire. During the 24 h recall interviews, each respondent reported the quantity of

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all foods and beverages consumed during the preceding day. To construct the food list for the

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Taiwan TDS, 268,431 raw data entries were first obtained from 6,104 questionnaires and then

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consolidated into 11,182 different food items which were grouped into 47 sub-categories and 12

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major categories on the basis of their nutrient content.34, 35 The number of food items selected from

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each sub-category for TDS was determined by the percentage of this sub-category in the total diet

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consumed. The second step involved determining which foods had the highest consumption rate

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(CR). The foods were ranked in the second step on the basis of percentage consumption, with 1% of

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the total diet being the cut-off rate. For example, the sub-category “rice and rice products”

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represented 10.4% of the amount of the total diet consumed daily; hence, the top 11 food items in

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this sub-category in descending order of CR were selected to represent this sub-category. In the

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third step, the amount of liquid food consumed was adjusted. The sub-categories “ice and 6

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beverages” and “soup,” where due to the large water content and relative uniformity of these food

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groups, the percentages of people consuming these groups (4.58 and 0.14%) instead of the

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percentages of amount consumed (29.80 and 10.72%) were used to keep the numbers of food items

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small. A total of 128 food items were selected from the 47 subcategories and 12 major categories to

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form a core list of food items to represent the total diet in Taiwan.

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Food list for TDS of preservatives. Not all food items contain preservatives. Only those

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containing high concentrations would have a significant contribution to health risk. Therefore, a

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food list specific to preservatives was constructed out of the core list of 128 items through the

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following adjustments. (1) Omitting from the core list the food items that were not likely to contain

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preservatives, such as fresh vegetables and fruits; (2) adding to the list the food items that were

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known to contain especially high levels of preservatives, including those known to frequently

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violate the preservative use regulations more than five times per year in the routine survey; (3)

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adding to the list the food items that were legally permitted to contain preservatives. Thus a

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preservative list of 97 food items from 47 sub-categories and 12 major categories was established,

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which was not totally dependent upon levels of daily intake rate. These 97 items were used as the

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basis for purchasing food samples to be prepared for chemical analysis of food preservatives.

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Purchasing of food samples and preparation of selected foods. From this list of 97, one to

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three food products were selected for collection and preparation of samples for chemical analysis.

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Consisted total of 239 food samples were obtained from 50 strategic sampling sites distributed

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among 4 cities and 4 counties in the northern, central, southern, and eastern parts of Taiwan. In each

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sampling site, food products were purchased from 5 wholesale stores, 9 supermarkets, and 24

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traditional wet markets. The purchased foods, food products, and food stuffs were combined,

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washed, cut, and cooked with flavoring agents according to standard recipes in the laboratory. For

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each item in the list of 97, at least eight products were purchased from the sampling sites, resulting

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in 2010 food products, which were used to prepare 239 food samples, including 46 cooked samples.

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These food samples were in turn used to prepare the 97 composite food samples for benzoic acid 7

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and sorbic acid analyses, by mixing equal weights of food products collected from all sampling sites

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in two seasons. Each composite sample was homogenized and stored at −80 °C until analysis. All

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analyses were carried out from 2010 to 2011.

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Analysis of preservatives. Analysis of food preservatives was conducted by first extracting

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benzoic acid and sorbic acid from 15 g of homogenized food matrix. Samples were extracted with

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150 mL of 50% methanol by shaking for 30 minutes, and then filtered. Deionized water was added

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to the filtrate to make up the volume to 250 mL, and the solution was filtered through a 0.45 µm

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membrane. The resulting extract was analyzed by high-performance liquid chromatography (HPLC)

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using a standard method (Chinese National Standards 10949-N6190). All chemicals used were of

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analytical reagent grade and the solvents were of HPLC grade. HPLC was performed by the

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Hungkuang University Testing and Analysis Center for Food and Cosmetics. This center has been

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certified for microbial, chemical, and genetic analyses of foods and cosmetics under International

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Organization for Standardization (ISO) 17025 guidelines.36 Chromatographic separation was

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performed using an Inertsil-ODS-2 (6 mm × 150 mm I.D.) analytical column, using

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methanol/acetonitrile/5 mM citric acid buffer (1:2:7, pH 4.0) as the mobile phase at a flow rate of 1

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mL/min. A diode array detector was used for analyzing chromatographically separated analytes, and

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detection was carried out at a wavelength of 230 nm. This method simultaneously measures the

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concentrations of five food preservatives, namely, benzoic acid, sorbic acid, dehydroacetic acid,

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salicylic acid, and alkyl p-hydroxy benzoates at a limit of quantification (LOQ) of 0.02 g/kg. Thus,

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the detected concentration was labeled as “ND” (not detected) when it is lower than 0.02 g/kg. The

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analysis was performed in duplicate, using blank, control, and spiked samples for quality control.

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The target recovery rate was between 80-120%; however, in cases wherein the recovery rate was

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below 80% and above 120%, the samples were retested.

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Estimation of average daily dose (ADD) of food preservatives. The ADD of benzoic acid or

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sorbic acid was calculated on the basis of the daily food consumption rate (CR) and the

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concentration (C) of benzoic acid or sorbic acid in food. 8

Thus ADD of an analyte in the total diet

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from food item i for the specified age group j is calculated as follows: n

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Ci × CRij (1) BWj i =1

ADDj = ∑

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where Ci is the concentration (mg/kg) of the analyte in food item i, CRij is the CR (g/person per day)

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of food item i by age group j, and BWj is the average BW of age group j. The data for C in diet

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samples, BW of various age groups, and CRs were obtained from the NAHSIT. According to the

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recommendation of the WHO, when C is less than the LOD, the chemical is to be reported as

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non-detected (ND). When the ND rate is less than 60%, the data were replaced by 1/2 LOD, and C

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values below the LOQ but above the LOD were replaced by 1/2 LOQ. If the ND rate were over

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60%, C values were assumed to be zero (ND).37

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In this study, the exposure groups were classified according to sex (male and female) and age

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as in NAHSIT. A total of 8 groups were classified by age and show the whole population. 8 groups

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included children of ages less than 1 year, 1-2 years, 3-6 years, 7-12 years, and 13-18 years; adults

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of ages 19-50 years and 51-65 years, individuals above 66 years old. The CRs of the 8 groups were

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estimated according to the 2005-2008 NAHSIT.33

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In the NAHSIT have been given a unique coding for each food, each of the codes follow the

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nutritional content of different foods, food type, type of processing, and other related properties, to

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reclassification of all food into 230 food items. In the 47 sub-categories (including 230 food items),

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sum of the amount of 11,182 available food intake records, we could get the total daily intake of all

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Taiwanese, and after converse we could obtained the daily intake. The daily intake in the

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questionnaire was corrected by weighting to adjust the national daily intake data by the following

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steps. (1) The questionnaire weight was the total population in the layer/number of samples in the

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layer; (2) The individual food daily intake was multiplied by the questionnaire weight to obtain the

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national daily intake; (3) National daily intake/number of the questionnaires in Taiwan and finally

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can get the food CR per person per day.

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Distributions of CR and BW values were analyzed by Monte Carlo simulation techniques to 9

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obtain probabilistic parameters such as percentile values, using the Crystal Ball® software available

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from Decisioneering, Inc., Denver, Co., USA. Probabilistic distributions of CR were fitted to the

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268,431 raw data obtained from 6,104 questionnaires. Distributions of the estimated BW of 8

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groups were fitted to the data obtained from 6,104 participants. The selected lognormal distributions

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of CR and normal distributions of BW have optimal χ2 fit and Kolmogorov–Smirnov (K–S)

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goodness-of-fit. Hazard index (HI, %ADI). The HI was calculated from the ADI and ADD according to the

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following equation: n

n

HIj = ∑ % ADI ij = ∑

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i =1

i =1

ADDij ADI P

n

× 100 % = ∑ i =1

Ci × CRij BW j × ADI P

× 100%

(2)

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where HIj is the hazard index for age group j and ADIp is the acceptable daily intake for chemical P.

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HI must be less than 100% to indicate that no harm would result from dietary exposure to the

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analyte in the lifetime of any consumer. ADIP is generally accepted as an intrinsic property of the

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target chemical P. Toxicological and ADI data, as well as hazard characterization data for benzoic

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acid and sorbic acid are collected from toxicological tests conducted on animals. ADI values of

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benzoic acid and sorbic acid used in this study were 5 mg/kg of BW/day and 25 mg/kg of BW/day,

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respectively, as promulgated by the JECFA.

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RESULTS AND DISCUSSION

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Concentrations of benzoic acid and sorbic acid. Representative food samples, collected in

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the fall and winter of 2010 and in the spring and summer of 2011, were analyzed to determine the

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concentration of preservatives. The purchased food samples detection rates for benzoic acid and

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sorbic acid were approximately 30% and 22% respectively, of the total samples analyzed. The

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method performance for benzoic acid and sorbic acid show in table 1. LOQ is 20 ppm and detected

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concentration is lower than 20 ppm will label as “ND”. In cases wherein the ND rate was greater 10

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than 60%, the concentration below the LOQ was assumed to be zero, and the concentrations of

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benzoic acid and sorbic acid were regarded as 0 mg/kg when calculating the daily intake.35 LOD is

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0.3 ppm considerably lower than that set by regulatory authorities in Taiwan. The analytical

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methods are in compliance with international standards for the analysis of food items in TDS

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requiring higher analytical sensitivities.38

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Preservative concentrations in major categories show in table 2. In the grains categories, 43

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samples were analyzed. Frequency of detection is 44.2% and mean concentration is 0.04 ppm in

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benzoic acid. Regulations pertaining to preservative use limit in Taiwan, the concentration of

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benzoic acid were 0.6 to 1.0 g/kg. In foods such as meats, sea urchins, caviar, peanut butter, cheese,

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candied fruits, dried fruits, dried radish containing no less than 25% moisture, cooked beans, miso,

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seaweed sauce, fermented bean curds, pastry, sauces, jam, juice, margarine, tomato sauce, chili

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sauce, thick candy syrup, and flavored syrup, the maximum permissible concentration is set at 1.0

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g/kg. For foods such as mullet roe, dried fish, dried shellfish, beverages, pickles, dried bean curd,

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and salted vegetables the maximum permissible concentration is set at 0.6 g/kg.

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About sorbic acid regulations limit concentration, add in food were 0.5 to 2.0 g/kg. For minced

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fish surimi products, meat products, urchins, caviar, peanut butter, soy sauce preserved vegetables,

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dried radish containing no less than 25% moisture, pickled vegetables, dried bean curd products,

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cheeses: not more than 2.0 g/kg calculated as sorbic acid. For cooked beans, soy sauces, miso, dried

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mullet roe, dried fish and shellfish products, seaweed pastes, soybean curd cheeses, syrup-

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preserved fruits, dried fruits, cakes and cookies (including steamed Chinese-styled ones), jams,

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juices, butter, cream, margarine, ketchup, chili sauces, fruit syrups, flavored syrups, other sauces:

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not more than 1.0 g/kg calculated as sorbic acid. Non-carbonated beverages, carbonated beverages

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the maximum permissible concentration is set at 0.5 g/kg.

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In our studies, the use of benzoic acid and sorbic acid as preservatives is permitted for only 34

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food items in Taiwan. Of the 239 food samples from two sampling seasons that were analyzed for

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preservatives, there are 90 food samples have little bearing on the 34 mentioned, even though the 11

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use of benzoic acid and sorbic acid as preservatives is permitted for only 34 food items, 46 out of

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the these 90 food samples (51%) were found to contain these preservatives. In addition, we found

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that the concentrations of benzoic acid in some samples of dried tofu, packaged dried tofu, bean

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pastes, and dried pickled radish were above the regulation limit. These findings suggest that the

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preservatives are widely distributed among foods other than the regulated 34 food items, making it

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imperative to regularly monitor the food industry in Taiwan.

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ADD of benzoic acid and sorbic acid. The ADD of food additives benzoic acid and sorbic

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acid in each item was estimated by measuring the concentration of the target chemical in the food

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sample. The results obtained by multiplying the concentration by the amount of food consumed are

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shown in table 3. To estimate the ADD of a target chemical consumed by a sex-specific and

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age-specific population using equation of ADD, data on the BW and the CR in 12 major categories

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of food were required. The exposure groups were classified according to 8 age groups of ages under

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1 year, 1-2 years, 3-6 years, 7-12 years, 13-18 years, 19-50 years, 51-65 years and over 66 years

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were estimated according to the 2005-2008 NAHSIT.33 The food list for the TDS, which was

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derived from the CR, contained 97 items selected to represent the total diet in Taiwan that may

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contain benzoic acid and sorbic acid. Items containing benzoic acid and sorbic acid that are

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consumed by the 8 age population were selected according to three selection criteria: (1) high

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relative CR; (2) historical high level of occurrence of the analytes; (3) items for which the use of the

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analytes is permissible. The food items in the TDS list represented 83% of the weight (g) of the total

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diet of general consumers in Taiwan.

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At the 50th percentile, males aged 1-2 years had the highest ADD of benzoic acid, with

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exposure level reaching 2.4 mg/kg of BW/day. In this group, the participators in 97 food items

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constituted 97.8% of a total of 184 people in the group, meaning that only 4 people did not intake

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these food items during the 24 h recall interviews. Females aged 3-6 years had the highest 95th

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percentile ADD of benzoic acid, with exposure level reaching 2.9 mg/kg of BW/day. The level of

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exposure to sorbic acid was 0.1 (under 1 year old group) to 0.7 (3-6 years old group) mg/kg of 12

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BW/day. Even at the 95th percentile, the exposure did not exceed 0.7 mg/kg of BW/day (3-6 years

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old group).

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HI (%ADI) of benzoic acid and sorbic acid. The HI values of benzoic acid and sorbic acid

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were calculated as a percentage of respective ADI, 5 and 25 mg/kg of BW/day, using equation (2).

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The ratio of ADD to ADI, taken as %ADI (figure 1 & figure 2), represents different exposure

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populations for benzoic and ascorbic acid. HI of benzoic acid and sorbic acid were calculated with

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the 50th percentile and 95th percentile of the different exposure populations.

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In figure 1, the food safety risk assessment %ADI show males aged 1-2 years (48.5%) and

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females aged 3-6 years (47.4%) at the 50th percentile had the highest %ADI of benzoic acid.

296

Whereas males (11.2%) and females (10.1%) aged 3-6 years had the highest %ADI for sorbic acid

297

at the 50th percentile show in figure 2. The values of HI for sorbic acid is generally lower than that

298

for benzoic acid. HI of benzoic acid and sorbic acid are below the ADI. At the 95th percentile, the

299

upper end of the intake distribution is still below the ADI; females over 66 years of age (61.7%) and

300

males 3-6 years of age (14.0%) had the highest %ADI for benzoic acid and sorbic acid, respectively.

301

These results indicate that there is a large margin of safety in the use of benzoic acid and sorbic acid

302

as food preservatives in Taiwan.

303

In a study carried out in Belgium, the daily intake of benzoic acid in the male population

304

exceeded the ADI (5 mg/kg of BW/day) at the 99th percentile, and the greatest contributor to the

305

intake was soft drinks.40 In our study, the ADD at the 99th percentile of men by all age groups did

306

not exceed the ADI. In a study in Finland, fruit and berry juices, soft drinks, and semi-preserved

307

fish were identified as the major sources of benzoic acid intake, with the exposure level being 40

308

mg/day, or 13% ADI.22 Comparing with the results of a 21st Australian TDS,13 the %ADI values for

309

benzoic acid and sorbic acid of our study were slightly higher than those in Australia at 50th

310

percentile, but lower at 95th percentile. Although the eating habits in Taiwan are markedly different,

311

the %ADI of benzoic acid and sorbic acid were nonetheless at very similar levels as in Australia.

312

Although the results of the Australia study show that the mean estimated dietary exposure to 13

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313

benzoates was less than 50%ADI for all population groups assessed, the 95th percentile estimated

314

dietary exposures to benzoates exceeded the ADI for young boys (approximately 140%) and young

315

girls (approximately 120%) aged 2-5 years.13 In the case of sorbates, the mean and 95th percentile

316

estimated dietary exposure were less than or equal to 40%ADI for sorbates for all population groups

317

assessed.

318

Our results indicate that the current exposure level to benzoic acid in foods in Taiwan is less

319

than 60% of the ADI, and hence not a hazard to public health. Combining the data for BW

320

distribution and food CRs obtained in this study, we determined the HI for the Taiwanese

321

population. The results indicate that in the 95th percentile, the exposure of the general population to

322

benzoic acid is less than 60% of the ADI and hence not at a harmful level. Benzoic acid and sorbic

323

acid are effective antimicrobials in acidic or slightly acidic foods. The temporary ADI was set at 5

324

mg/kg of BW by the European Scientific Committee on Food in 1994. The JECFA set an ADI of 5

325

mg/kg of BW in 1996, which was a confirmation of the evaluation in 1994. The 100-fold SF built

326

into the ADI provides a significant margin of safety, which serves to reduce the likelihood of

327

adverse effects on humans. As the %ADI is not over 100%, we assume that under the current

328

exposure scenario, benzoic acid and sorbic acid pose no significant food safety risk in Taiwan.

329

However, HIs even as high as 48.5%ADI (male 1-2 years group) at the 50th percentile, suggesting

330

that regulatory actions must be implemented.41

331

HI (%ADI) exposure contributor for benzoic acid and sorbic acid. The intake of benzoic

332

acid and sorbic acid through various food groups by various age groups is shown in figures 3 and 4.

333

According to the HI (%ADI) results, the 0-6 age sensitive population might have a higher risk of

334

exposure to benzoic acid or sorbic acid. However, using adult food to estimate the infant (0-2 years

335

old) dietary exposure would be an overestimation. Therefore, we focused on high-risk sensitive

336

population aged 3-6 years and general population aged 19-50 years to explore further the exposure

337

contributor of preservatives benzoic acid and sorbic acid (figures 3 and 4). In 3-6 years population,

338

the main HI contributors for benzoic acid were sausage (28.6%) for male and seasonings (31.8%) 14

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for female, respectively. The main HI contributors for sorbic acid were pork products (39.4%) for

340

male and cakes (25.8%) for female, respectively. In 19-50 years population, the main HI

341

contributors for benzoic acid were dumplings and pot stickers (21.8%) for male and seasonings

342

(34.5%) for female. The main HI contributors for sorbic acid were beef (29.5%) for male and cakes

343

(23.7%) for female. Seasonings like tomato sauce, chili sauce and soy sauce are added benzoic acid

344

as a preservative to protect it from going bad. Dumpling and pot sticker skin were foods with high

345

moisture that promotes growth of mold, yeast and bacteria, whereas adding benzoic acid can inhibit

346

them. Sorbic acid and its salts are used to protect cakes against mold spoilage and as inhibitors of

347

Clostridium botulinum in meat products in order to replace the use of nitrites, which produce

348

carcinogenic nitrosamines.

349

In a study of dietary exposure to benzoic acid in secondary school students by Ma et al.,15 the

350

dietary exposures for average and high consumers of the school students from prepackaged

351

beverages were 0.31 and 0.97 mg/kg BW per day, respectively. Both exposure levels were below

352

the ADI established by JECFA. However, in the worst-case scenario where consumers had specific

353

brand loyalty towards the fruit juice sample with the highest benzoic acid level detected in the study

354

15

; the general exposure in high consumers would exceed the ADI, leading to increased health risk.

355

In comparison, the major HI contributors for benzoic acid and sorbic acid in Australia were

356

beverages (soft drinks) and fresh juices, 13 reflecting the vast difference in eating habits between the

357

Orientals and the Caucasians. Likewise, in the Belgian study, the male group aged 15 years and

358

older had a higher intake of benzoic acid than females due to a higher intake of soft drinks; their

359

99th percentile exposure exceed the ADI.40 By conservative assessment of daily exposure, we found

360

that seasoning, dumplings and pot stickers were identified as the major sources of benzoic acid

361

intake in Taiwan and hence require continuous monitoring.

362

Uncertainty analysis. There are some methodological limitations and uncertainties in our

363

study that need to be noted. First, Chinese foods are complex and dynamic, and it is very difficult to

364

exactly match the food groups or items to be surveyed with the foods actually consumed. Second, 15

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foods analyzed in this survey were originally mapped to a wider range of foods described in the

366

NAHSIT for a different research purpose, as the patterns of preservatives used in the mapped foods

367

were assumed to be similar to the 97 food items analyzed, a kind of uncertainty inevitably was

368

introduced. Third, it followed that the ADDs of preservatives were estimated with exposure factors

369

associated with only these 97 items, introducing another kind of uncertainty. These uncertainties

370

may cause underestimation. However, with our selection criteria, we believed that all the major

371

sources of foodborne preservatives were covered. We also assessed the %ADI at the 95th percentile

372

in order to avoid underestimation. In addition, the dietary exposures to benzoic acid and sorbic acid

373

might have been overestimated in 1 year and 1-2 years, since these groups are infants who consume

374

mainly milk or baby food which are inherently different from adult food. Further studies will be

375

conducted to examine this issue further. Finally, the one-day 24 h dietary recall records from the

376

NAHSIT undoubtedly contained another kind of uncertainty due to individual differences in daily

377

dietary practice. Our study therefore represents a preliminary attempt to construct a “market basket”

378

for the total diet in Taiwan. To improve the accuracy of our estimates, future efforts are focused on

379

minimizing the above-mentioned uncertainties and on validating the models and values of exposure

380

factors in utilizing the data resources from NAHSIT, a major national research investment in

381

Taiwan. In conclusions, the purpose of this study was to evaluate the HI (%ADI) of benzoic acid

382

and sorbic acid through ingestion and thereby establish a model for total diet study on food

383

additives in Taiwan by utilizing the existing data available from a national nutritional status survey,

384

NAHSIT. The calculated 95th percentile ratios of ADD to ADI of benzoic acid and sorbic acid were

385

less than 60 %ADI, suggesting that the use of the two preservatives in food in Taiwan is within safe

386

limits. This study provides a model for future work to address specific additives in specific foods as

387

needed by food safety risk regulatory agencies.

388

In conclusion, this study demonstrated a dietary exposure estimates for the food preservatives

389

benzoic acid and sorbic acid in the total diet in Taiwan (figure 5). In hazard identification, related

390

research in total diet study and the physical and chemical properties of preservatives benzoic acid

391

and sorbic acid were collected. Then, in exposure analysis, ADD was estimated with Monte Carlo 16

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simulation. In hazard characterization, ADI, toxicological data (e.g., NOEL) and SF of the

393

preservatives from international institutions such as JECFA were analyzed. The dose-response

394

profile was estimated according to the ADI by the JECFA. Lastly, in risk characterization, the

395

probability distribution of the food safety risk was estimated and compared to ADI. In high-intake

396

consumers, the highest HI of benzoic acid was 61.7 %ADI for females aged over 66 years old. The

397

highest HI of sorbic acid for male and female consumers aged 3-6 years old at the 95th percentile

398

were 14.0 %ADI and 12.2 %ADI, respectively. These results indicate that the use of benzoic acid

399

and sorbic acid as preservatives at the current level of use in the Taiwanese diet does not constitute

400

a public health and safety concern. But the public is advised to maintain a varied and balanced diet

401

so as to avoid excessive exposure of benzoic acid and sorbic acid from a small range of food items.

402

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403

ABBREVIATIONS USED

404

ADD, average daily dose; ADI, acceptable daily intake; BW, body weight; C, concentration;

405

CR, consumption rate; GEMS/Food, Global Environment Monitoring System-Food Contamination

406

Monitoring and Assessment Program; HI, hazard index; HPLC, high-performance liquid

407

chromatography; ISO, International Organization for Standardization; JECFA, Joint FAO/WHO

408

Expert Committee on Food Additives; LOD, limit of detection; LOQ, limit of quantification;

409

NAHSIT, Nutrition and Health Survey in Taiwan; ND, not detected; NOEL, no observed effect

410

level; SF, Safety Factor; TDS, total diet study; TFDA, Taiwan Food and Drug Administration; WR,

411

weight ratio

412 413

ACKNOWLEDGMENTS

414

This TDS project was financed by the Taiwan Food and Drug Administration (TFDA),

415

Department of Health (DOH), contract TFDA-TC-103. The data on related exposure factors,

416

including BW and CR, were kindly provided by Dr. W. H. Pan, Principal Investigator of the

417

National NAHSIT sponsored by the DOH (DOH94-FS-6-4). The authors wish to thank our project

418

manager at TFDA, and the many food safety colleagues in Taiwan and TDS experts in China and

419

elsewhere for their generous and professional help in completing this project. Without the help, we

420

would not have been able to carry out this study. We would especially like to acknowledge the

421

leadership and important contributions of co-author DPHH, who has now honorably retired.

422

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REFERENCES

424

(1) Penninggton, J.A.T.; Gunderson, E.L. History of the Food and Drug Admintration’s Total Diet

425 426

Study-1961 to 1987. J. AOAC Off. Anal. Chem. 1987, 70, 772-782. (2) WHO/FAO

(World

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and

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Organization).Codex

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alimentarius commission procedural manual. 20th ed. 2011, pp. 112. Joint FAO/WHO Food

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Standards Programme, FAO, Rome.

429

(3) EFSA (European Food Safety Authority). Joint Guidance of EFSA, FAO and WHO. Towards a

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harmonised Total Diet Study approach: a guidance document. EFSA J. 2011, 9(11), 2450.

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(4) Moy, G.G. Total Diet Studies. 1st ed. Springer, 2011; pp. 1-400.

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(5) EFSA (European Food Safety Authority). Technical Report of EFSA, FAO and WHO. State of

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the art on Total Diet Studies based on the replies to the EFSA/FAO/WHO questionnaire on

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national total diet study approaches, 2011.

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(6) Cunningham, W.C.; Anderson, D.L.; Baratta, E.J. Radionuclides in domestic and imported foods in the United States, 1987-92. J. AOAC Int. 1994, 77, 1422-1427.

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(7) Chen, H.L.; Su, H.J.; Hsu, J.F.; Liao, P.C.; Lee, C.C. High variation of PCDDs, PCDFs, and

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dioxin like PCBs ratio in cooked food from the first total diet survey in Taiwan. Chemosphere

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(8) Li, X.W.; Gao, J.Q.; Chen, J.S. Chinese total diet study in 2000: the dietary mercuric intakes. Wei Sheng Yan Jiu (Journal of Hygiene Research), 2006, 3, 323-325.

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(9) Leblanc, J.C.; Tard, A.; Volatier, J.L.; Verger, P. Estimated dietary exposure to principal food

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mycotoxins from the first French Total Diet Study. Food Addit. Contam. 2005, 22, 652-672.

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(10) Ministry of Agriculture and Forestry (MAF), 2009 New Zealand Total Diet Study Agricultural

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compound residues, selected contaminant and nutrient elements. Ministry of Agriculture and 19

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Forestry, Wellington, 2011. (11) FSANZ (Food Standards Australia New Zealand). The 22nd Australian Total Diet Study. A total diet study of five trace elements: iodine, selenium, chromium, molybdenum, and nickel, 2008. (12) Tfouni, S.A.; Toledo, M.C. Estimates of the mean per capita daily intake of benzoic and sorbic acids in Brazil. Food Addit. Contam. 2002, 19, 647-654. (13) FSANZ (Food Standards Australia New Zealand). The 21st Australian Total Diet Study-A total diet study of sulphites, benzoates and sorbates, 2005. (14) Leth, T.; Christensen, T.; Larsen, I.K. Estimated intake of benzoic and sorbic acids in Denmark. Food Addit. Contam. 2010, 27, 783-792.

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(15) Ma, K.M.; Chan, C.M.; Chung, S.W.; Ho, Y.Y.; Xiao, Y. Dietary exposure of secondary school

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students in Hong Kong to benzoic acid in prepackaged non-alcoholic beverages. Food Addit.

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Contam. 2009, 26(1), 12-6.

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(16) Lino, C.M.; Pena, A. Occurrence of caffeine, saccharin, benzoic acid and sorbic acid in soft

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drinks and nectars in Portugal and subsequent exposure assessment. Food Chem. 2010, 121,

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(17) WHO (World Health Organization). GEMS Food total diet studies report of the 3rd international workshop on total diet studies. WHO, Geneva. 2004.

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(18) Suhr, K.I.; Nielsen, P.V. Effect of weak acid preservatives on growth of bakery product

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spoilage fungi at different water activities and pH values. Int. J. Food Microbiol. 2004, 95,

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(19) European Union, European Parliament and Council Directive No. 95/2/EC of 20 February 1995 on food additives other than colours and sweeteners. Off. J. Eur. Union, 1995, 61, 1-40.

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(20) Taiwan Food and Drug Administration (TFDA). Standards for Specification, Scope,

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Application and Limitation of Food Additives List, http://www.fda.gov.tw/EN/law.aspx 20

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(accessed May 19, 2014). (21) Taiwan Food and Drug Administration (TFDA). Annual Report of Food and Drug Research, http://www.fda.gov.tw/TC/PublishResearch.aspx (accessed May 19, 2014). (22) Pentilla, L.; Salminen, S.; Niemi, E. Estimates on the intake of food additives in Finland. Z. Lebensm. Unters. Forsch. 1988, 186, 11-15.

(23) Kieckebusch, W.; Lang, K. The tolerability of benzoic acid in chronic feeding experiments. Arzneimittelforschung. 1960, 10, 1001-1003 .

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(24) McCann, D.; Barrett, A.; Cooper, A.; Crumpler, D.; Dalen, L.; Grimshaw. K.; Kitchin, E.; Lok,

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K.; Porteous, L; Prince, E.; Sonuga-Barke, E.; Warner, J.O.; Stevenson, J. Food additives and

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hyperactive behavior in 3-year-old and 8/9-year-old children in the community: a randomised,

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double-blinded, placebo-controlled trial. Lancet 2007, 370, 1560-1567.

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(25) USEPA (U.S. Environmental Protection Agency). Guidelines for Developmental Toxicity Risk Assessment. Federal Register 1991, 56, 63798-63826. (26) Renwick, A.G. Safety factors and establishment of acceptable daily intakes. Food Addit Contam. 1991, 8, 135-149.

(27) Sado, I. Synergistic toxicity of official permissible preservative food additives. Nippon Eiseigaku Zasshi (Japanese Journal of Hygiene), 1973, 28, 463-476.

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(28) Lang, K. The tolerability of sorbic acid. Arzneimittelforschung. 1960, 10, 997-999.

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(29) Walker, R. Toxicology of sorbic acid and sorbates. Food Addit. Contam. 1990, 7(5), 671-6.

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(30) Deuel, H.J.; Alfin-slater, R.; Well, C.S.; Smyth, H.F. Sorbic acid as a fungistatic agent for

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foods. Food Res. 1954, 19, 1.

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(31) JECFA (Joint FAO/WHO Expert Committee on Food Additives). Evaluation of certain food

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additives and contaminants. Forty-sixth report of the Joint FAO/WHO Expert Committee on 21

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Food Additives. WHO Technical Report Series No. 868. WHO, Geneva. 1996.

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(32) WHO (World Health Organization). Benzyl Acetate, Benzyl Alcohol, Benzaldehyde, Benzoic

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Acid and the Benzoate Salts, Forty Sixth Report of the Joint FAO/WHO Expert Committee on

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Food Additives, WHO Technical Report Series No. 868. WHO, Geneva. 1997.

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(33) Pan, W.H. Nutrition and Health Survey in Taiwan 2004-2008. Project Report, DOH94-FS-6-4. Food and Drug Administration, Department of Health, Taiwan, R.O.C. 2008. (34) Egan, S.K.; Bolger, P.M.; Carrington, C.D. Update of US FDA’s Total Diet Study food list and diets. J. Expo. Sci. Environ. Epidemiol. 2007, 17(6), 573-582.

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(35) Egan, S.K.; Tao, S.S.; Pennington, J.A.; Bolger, P.M. US Food and Drug Administration’s

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Total Diet Study: intake of nutritional and toxic elements 1991-96. Food Addit. Contam. 2002,

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19(2), 103-125.

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(36) ISO, ISO 17025. General requirements for the competence of testing and calibration laboratories, 2005.

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(37) WHO (World Health Organization). Principles and methods for the risk assessment of

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chemicals in food: Chapter 6 dietary exposure assessment of chemicals in food. Environmental

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Health Criteria, 2009, 240, 19-21.

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(38) US FDA. Pesticide Monitoring Program - FY 2008, anual report, 2008.

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(39) JECFA (Joint FAO/WHO Expert Committee on Food Additives). Seventeenth Report of the

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Joint FAO/WHO Expert Committee on Food Additives. WHO Technical Report Series No. 539.

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WHO, Geneva. 1973.

513

(40) Vandevijvere, S.; Andjelkovic, M.; De, Wil, M.; Vinkx, C.; Huybrechts, I.; Van, Loco, J.;

514

VanOyen, H.; Goeyens, L. Estimate of intake of benzoic acid in the Belgian adult population.

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Food Addit. Contam. 2009, 7, 958-968.

516

(41) CAC (Codex Alimentarius Commission). Procedural manual. Codex Committee on Food 22

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517

Additives and Contaminants (CCFAC) guidelines for exposure assessment of contaminants

518

and toxins in food or food groups. 15th Ed., 2013.

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Table 1. Method performance for Benzoic acid and sorbic acid. Measurement Accreditation uncertainty Yes/No (ppm)

LOQ (ppm)

Recovery range (%)

RSD (%) (n= 5)

Benzoic acid Meat product

20

96.7±1.90

1.76

250.0±1.2

yes

Sorbic acid Meat product

20

97.1±1.07

1.26

250.0±1.2

yes

Analyte

Matrix

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Table 2. Preservative concentrations in food samples. No. of analysis Major categories of food Preservative performed

Frequency of Mean concentration detection (%) ±SD (ppm)

Benzoic acid

43

44.2

0.04±0.07

Sorbic acid

43

34.9

0.04±0.08

Benzoic acid

4

25.0

0.02±0.04

Sorbic acid

4

25.0

0.07±0.14

Benzoic acid

7

28.6

0.02±0.03

Sorbic acid

7

14.3

0.02±0.06

Benzoic acid

17

35.3

0.06±0.13

Sorbic acid

17

47.1

0.21±0.35

Benzoic acid

11

36.4

0.05±0.08

Sorbic acid

11

45.5

0.09±0.15

Benzoic acid

43

62.8

0.2±0.33

Sorbic acid

43

23.3

0.1±0.29

Benzoic acid

6

16.7

0.06±0.16

Sorbic acid

6

33.3

0.05±0.08

Benzoic acid

16

68.8

0.53±0.94

Sorbic acid

16

31.3

0.05±0.09

Benzoic acid

49

10.2

0.01±0.02

Sorbic acid

49

14.3

0.04±0.19

Benzoic acid

2

0.0

-

Sorbic acid

2

0.0

-

Benzoic acid

20

30.0

0.13±0.28

Sorbic acid

20

10.0

0.01±0.02

Benzoic acid

21

19.0

0.03±0.08

Sorbic acid

21

14.3

0.05±0.16

1 Grains

2 Oils

3 Poultry and poultry products

4 Meat and meat products

5 Fish and aquatic products

6 Other proteins

7 Fruits (processed)

8 Vegetables (processed)

9 Dessert

10 Alcoholic beverages

11 Seasonings

12 Others

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Table 3. ADD of food preservatives for various exposure populations. Participators Exposure Whole (%) in 97 food Benzoic acid population participators items 50th ADD a Age group Under 1 Yr.

Male

Female

Male

Sorbic acid

95th ADD

50th ADD

95th ADD

Female Male

Female

Male

Female

Male

Female

Male

Female

73

67

67.1

71.6

0.2

0.1

0.2

0.1

0.1

0.1

0.1

0.1

1–2 Yr.

184

170

97.8

98.2

2.4

1.5

2.7

1.9

0.5

0.4

0.6

0.5

3–6 Yr.

466

483

100.0

99.8

1.6

2.4

1.9

2.9

0.6

0.5

0.7

0.6

7–12 Yr.

1170

1018

99.9

100.0

1.5

1.0

1.8

1.1

0.3

0.2

0.3

0.2

13–18 Yr.

713

729

99.9

99.3

1.0

0.9

1.5

1.2

0.2

0.2

0.5

0.3

19–50 Yr.

1062

1082

100.0

99.9

1.0

1.2

1.7

2.0

0.2

0.2

0.4

0.5

51–65 Yr.

539

536

99.6

99.3

0.9

0.9

1.5

1.6

0.2

0.1

0.3

0.3

Over 66 Yr.

720

722

99.2

98.1

1.2

1.2

2.4

3.1

0.2

0.2

0.4

0.4

Over 3 Yr.

4670

4570

99.8

99.5

1.1

1.2

2.1

2.4

0.3

0.2

0.5

0.4

a

ADD: average daily dose of food preservatives (mg/kg bw/day).

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60

Male 50

%ADI

40

30

20

10

0 66

Age (year-old) 70

Female 60

50

%ADI

40

30

20

10

0 66

Age (year-old)

Figure 1. The food safety risk assessment hazard index (%ADI) of benzoic acid. 27

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16

Male 14

12

%ADI

10

8

6

4

2

0 66

Age (year-old)

14

Female 12

10

%ADI

8

6

4

2

0 66

Age (year-old)

Figure 2. The food safety risk assessment hazard index (%ADI) of sorbic acid. 28

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(A) Benzoic acid Male 3-6 yr.

Female 3-6 yr.

(B) Sorbic acid Male 3-6 yr.

Female 3-6 yr.

Figure 3. Exposure contributor of preservatives benzoic acid and sorbic acid for male and female aged 3-6 years old.

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(A) Benzoic acid Male 19-50 yr.

Female 19-50 yr.

Male 19-50 yr.

Female 19-50 yr.

(B) Sorbic acid

Figure 4. Exposure contributor of preservatives benzoic acid and sorbic acid for male and female aged 19-50 years old.

30

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Figure 5. Flowchart of dietary exposure estimates for the food preservatives benzoic acid and sorbic acid in the total diet in Taiwan.

31

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