Food Additives & Contaminants

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Food Additives & Contaminants


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Estimated daily intakes of butylated hydroxyanisole


(BHA), butylated hydroxytoluene (BHT) and tert-butyl
hydroquinone (TBHQ) antioxidants in Korea
a a a a a a
H.-J. Suh , M.-S. Chung , Y.-H. Cho , J.-W. Kim , D.-H. Kim , K.-W. Han & C.-J. Kim
b

a
Korea Health Industry Development Institute , 57-1 Noryangjin-Dong, Dongjak-Ku, Seoul
156-800, Korea
b
Department of Food & Nutrition , Sook Myung Women's University , 53-12, Chungpa-Dong 2
Ga, Yong San-Ku, Seoul 140-742, Korea
c
Department of Food & Nutrition, Sook Myung Women's University , 53-12, Chungpa-Dong 2
Ga , Yong San-Ku, Seoul 140-742, Korea E-mail:
Published online: 16 Feb 2007.

To cite this article: H.-J. Suh , M.-S. Chung , Y.-H. Cho , J.-W. Kim , D.-H. Kim , K.-W. Han & C.-J. Kim (2005) Estimated daily
intakes of butylated hydroxyanisole (BHA), butylated hydroxytoluene (BHT) and tert-butyl hydroquinone (TBHQ) antioxidants
in Korea, Food Additives & Contaminants, 22:12, 1176-1188, DOI: 10.1080/02652030500195288

To link to this article: http://dx.doi.org/10.1080/02652030500195288

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Food Additives and Contaminants, December 2005; 22(12): 1176–1188

Estimated daily intakes of butylated hydroxyanisole (BHA), butylated


hydroxytoluene (BHT) and tert-butyl hydroquinone (TBHQ)
antioxidants in Korea

H.-J. SUH2, M.-S. CHUNG1, Y.-H. CHO1, J.-W. KIM1, D.-H. KIM1, K.-W. HAN1, & C.-J. KIM2
1
Korea Health Industry Development Institute, 57-1 Noryangjin-Dong, Dongjak-Ku, Seoul 156-800, Korea and
2
Department of Food & Nutrition, Sook Myung Women’s University, 53-12, Chungpa-Dong 2 Ga, Yong San-Ku,
Seoul 140-742, Korea

(Received 7 February 2005; revised 21 September 2005; accepted 21 September 2005)


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Abstract
The study was conducted to establish the estimated daily intake (EDI) of antioxidants such as butylated hydroxyanisole
(BHA), butylated hydroxytoluene (BHT) and tert-butyl hydroquinone (TBHQ) in Korea. The EDIs were obtained from two
sources. One of the estimations was based on the analytical determination of BHA, BHT and TBHQ in 12 food categories
(ten food categories for TBHQ) and on individual dietary intake data obtained from the National Health and Nutrition
Survey in 1998 (n ¼ 11 525, age > 1 year). The other EDIs of BHA, BHT and TBHQ were based on the maximum permitted
levels specified in national food standards in Korea and on individual dietary intake data obtained from the National Health
and Nutrition Survey in 1998 (n ¼ 11 525, age > 1 year). To establish the EDIs based on the analytical determination and on
individual dietary intake data, 133 food samples in 12 food categories were selected from the foods considered to be
representative sources of BHA, BHT and TBHQ in the Korean diet. Selected samples were analysed by GC with FID. BHA
was not detected in any of the samples analysed. BHT and TBHQ were detected in the samples, but the levels were
significantly lower than their maximum limits. The EDIs1 of BHT, and TBHQ for average consumers were 0.01563, and
0.00123 mg kg1 body weight bw day1 and as a proportion of the ADI were 0.0052 and 0.0002%, respectively. For 95th
percentile consumers, the EDIs of BHT and TBHQ were 0.0080 and 0.0006 mg kg1 bw day1, and as a proportion of the
ADI were 2.67 and 0.09%, respectively. EDIs for BHA, BHT and TBHQ based on the maximum permitted levels and on
individual dietary intake data were 0.04, 0.04 and 0.04 mg kg1 bw day1, respectively. The EDIs of BHA, BHT and TBHQ
for average consumers ranged from 6.00 to 14.42% of the ADI of each antioxidant. According to these results, the EDIs of
BHA, BHT and TBHQ in Korea were significantly lower than ADI of these antioxidants established by the JECFA.

Keywords: Estimated daily intake (EDI), antioxidants, BHA, BHT, TBHQ

Introduction human, animal or plant life or health, taking into


account risk assessment techniques developed by
Food additives are edible ingredients deliberately
the relevant international organizations.
used in food processing and production. However,
when abused or misused, they may affect and harm Each country has performed risk assessment of food
human health. Due to this fact, the safety manage- additives, taking the assessment models developed by
ment of food additives is very important. Article 5 of the Codex Committee for Food Additives and
the Agreement on Sanitary and Phytosanitary Contaminants (CCFAC) into consideration.
Measure (SPS) of the World Trade Organization CCFAC has provided the procedures and the
stipulates as such: guidelines on daily intake assessment of food
additives and recommended each country should
members shall ensure that their sanitary or follow those. When many countries set up the
phytosanitary measures are based on assessment, standard for food additives, they established regula-
as appropriate to the circumstances, of the risks to tions for securing the safety, considering factors such

Correspondence: M.-S. Chung. E-mail: chungms@khidi.or.kr


ISSN 0265–203X print/ISSN 1464–5122 online ß 2005 Taylor & Francis
DOI: 10.1080/02652030500195288
Estimated daily intakes of BHA, BHT and TBHQ antioxidants in Korea 1177

as daily intakes of food additives and the appropriate economic surveys or retail sales surveys, from 0.02
use level of food additives representing technical to 0.09 mg kg1 bw (except for the USA) based on
effects on toxicity expected from food additives, model diets (for consumers with average intakes),
manufacturing, processing, preparation, treatment, and from 0.02 to 0.1 mg kg1 bw based on individual
packing, packaging and transporting or holding of dietary records.
foods (Codex Alimentarius 1995). The Committee noted the following two excep-
To use food additives safely, the CCFAC has tions. The first was that the estimates of daily per
drawn special attention to phenolic antioxidants such capita intake based on a model diet and the
as BHA, BHT and TBHQ. In this respect, recently maximum permitted level of use of BHT in the
the Joint Expert Committee of Food Additives USA were 0.39 and 0.78 mg kg1 bw for mean and
(JECFA) assessed the intake level of BHA and high levels of consumption, respectively. This result
BHT among ten Member States: Australia, Brazil, can be explained by the high maximum permitted
China, Finland, France, Japan, New Zealand, Spain, level of use of BHT in the USA. The second
the UK and the USA. The intake level of TBHQ was exception was a study from Japan, which was based
assessed for six Member States (Australia, Brazil, on analytical results for BHT from a market basket
China, New Zealand, the UK and the USA) of survey. The estimate of daily per capita intake
CODEX during its 51st meeting. According to the (0.00085 mg kg1 bw) was lower than all the other
WHO meeting report, all the national assessments of intake estimates submitted.
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intake of BHA, BHT and TBHQ evaluated by the National intake estimates of TBHQ based on
committee, except that from Japan, were based on maximum limits specified in the draft General
the use of food additives at the maximum limits Standard for Food Additives submitted by only five
specified in the draft General Standard for Food Member States. The estimates of mean intake of
Additives, maximum limits specified by the TBHQ ranged from 90% of the ADI for the USA to
European Union, or maximum limits specified in 180% of the ADI for Australia and New Zealand
national food standards (WHO 2000). (combined). All the best estimates of national mean
National estimates of mean intake of BHA based intake of TBHQ ranged from 50% of the ADI for
on maximum limits specified in the draft General the USA to 100% of the ADI for China, based on
Standard for Food Additives were submitted by only model diets or individual dietary records. Intake
three Member States. The estimates of mean intake estimates for consumers with high intakes of TBHQ
ranged from 180% of the ADI for Australia and based on maximum limits specified in national food
New Zealand (combined) to 190% of the ADI for standards exceed the ADI in some cases (e.g. 300%
the USA. National estimates of mean intake for for Australia and New Zealand (combined)).
consumers of BHA based on maximum limits However, the data submitted were insufficient to
specified in national food standards or by the estimate the number of such consumers or the
European Union ranged from 1% of the ADI for magnitude and duration of intake above the ADI
Japan to 80% of the ADI for Australia and (WHO 2000).
New Zealand (combined) and the USA. These In Korea, the National Institute of Health (NIH)
estimates were based either on model diets or on and the Korea Food and Drug Administration
individual dietary records submitted by seven (KFDA) had performed the monitoring on phenolic
Member States (Australia and New Zealand (com- antioxidants in 1985, 1991 and 1998, respectively,
bined), China, France, Japan, the UK and the USA). and those monitoring practices were intended to
Intake estimates for consumers with high intakes of establish the experimental method. The study by
BHA based on maximum levels of food additives Yoon et al. (1991) was the first on daily intake
specified in national standards ranged from 30% of assessment using budget methods. EDIs of BHA,
the ADI for France to 260% of the ADI for Australia BHT and TBHQ by the Budget method were
and New Zealand (combined). calculated based on use level of those antioxidants
National estimates of daily per capita intake of and Budget factor. According to Yoon et al., daily
BHT based on maximum limits specified in the draft intakes of BHA, BHT and TBHQ in Korea were
General Standard for Food Additives ranged from 3.588, 3.588 and 2.31 mg kg1 bw day1, respec-
0.70 to 0.99 mg kg1 bw for consumers with mean tively, and exceeded the acceptable daily intake
intakes and from 2.0 to 6.0 mg kg1 bw day1 for (ADI). Therefore, except that by the budget
consumers with high intakes. method, using other assessment methods proposed
Intake estimates of daily per capita intake of by the JECFA, this study was conducted to evaluate
BHT based on maximum limits specified in the estimated daily intakes (EDIs1) of antioxidants
national food standards ranged from 0.003 to such as butylated hydroxyanisole (BHA), butylated
0.11 mg kg1 bw based on ‘poundage’ data, from hydroxytoluene (BHT) and tert-butyl hydroquinone
0.052 to 0.1 mg kg1 bw based on household (TBHQ) by coupling the concentrations of these
1178 H.-J. Suh et al.

three antioxidants in foods and individual dietary The content of BHA, BHT and TBHQ in foods
intake data from the National Nutrition Survey in has been monitored for the last several years in Korea
1998, as well as the estimated daily intake (EDIs2) (Kim et al. 1985, 1991). According to the previous
of these three antioxidants based on the maximum studies, the detection rates of these antioxidants in
permitted levels of antioxidants specified in national foods differ. It is much greater probability to detect
standards in Korea and on individual dietary the antioxidants from foods showing a higher
intake data. detection rate based on previous studies than those
showing a lower detection rate. Due to this fact, the
food samples for estimated daily intake of BHA,
Materials and methods BHT and TBHQ were selected by a stratified
random sampling method employing detection rate
Sampling plan and determination of antioxidants
obtained from previous studies as a stratum (Kim
Table I shows the maximum permitted levels et al. 1985, 1991). The results of the detection rate
(MPLs) and the range of foods of BHA, BHT and for the same food sample in the above two studies
TBHQ specified in national food standards in Korea have used the most recent data set. This method is
(KFDA 1999a). A stepwise procedure was used in frequently used for stratified random sampling in all
this study to select food categories for estimating the surveys. It is called proportional allocation that the
daily intake of BHA, BHT and TBHQ. At the first size of the sample in each stratum is taken in
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tier of selecting procedure of food categories, proportion to the size of the stratum (Scheaffer
12 food group shown in Table I were considered to et al. 1990).
estimate the daily intake of these antioxidants but The total sample numbers for the analysis of
both instant food and poultry among the 12 food BHA, BHT and TBHQ were determined
groups were excepted from this study because BHA according to:
and BHT had not been detected in previous studies
(Kim et al. 1985). So, ten food groups such as oil, Di
na ¼ P  100  TN ð1Þ
tallow, lard, butter, dried fishery product, salted Di
fishery product, frozen fishery product, chewing
gum, breakfast cereal and mayonnaise were where na is the sample numbers of the specific ‘a’
considered to estimate the daily intake of these food category, Di is the previous detection rate (%)
antioxidants. of antioxidants in the specific food categories and
At the second tier, 12 food categories such as TN is the total number of samples supposed to be
soybean oil, corn oil, other vegetable oil, shortening, analysed for the specific ‘a’ antioxidants.
margarine, seasoned dried fish, dried fish, salted The samples in all food categories were purchased
fishery product, frozen fishery product, chewing by stratified random sampling basis of market share
gum, mayonnaise, and breakfast cereal among information (KFDA, 1999a). The half of the samples
those ten food groups were selected and to determine in each food category were from the companies in the
which were considered to be representative sources top 25% of market shares, 30% of samples were from
of BHA, BHT and TBHQ in the Korean diet. the companies in the middle 50% of market share.
The other 20% of samples were from the companies
in the lowest 25% of market share (Table II).
Table I. Technical regulations for BHA, BHT and TBHQ
All of the sampling design employed by Yoon et al.
in Korea.
and more detailed information related sampling
Permitted design are described in Yoon et al. (2001, 2003).
Antioxidants Application level (g kg1)
BHA  BHT Oil, tallow, lard, butter, <0.2
dried fishery product, GC analyses for the antioxidants
salted fishery product
Frozen fishery product, <1 Standards and internal standard such as benzo-
salted frozen whale meat phenone were purchased from Sigma Chemical Co.
Chewing gums <0.75 (St Louis, MO, USA) for the analysis of BHA, BHT
Breakfast cereal, instant food <0.05 and TBHQ. TBA-OH was obtained from Acros
Mayonnaise <0.14 (BHT:0.06)
Organics (Geel, Belgium). Acetonitrile, n-pentane,
Poultry <0.01
TBHQ Oil, tallow, lard, butter, <0.2 dichloromethan and ammonium hydroxide were
dried fishery product, obtained from Junsei Chemical Co. (Tokyo, Japan).
salted fishery product The extraction procedure for the determination
Frozen fishery product, <1.0 of BHA, BHT and TBHQ in this study was
salted frozen whale meat
performed by the AOAC official Method 983.15
Chewing gums <0.75
for Phenolic Antioxidants in Oil, Fats, and Butter Oil
Estimated daily intakes of BHA, BHT and TBHQ antioxidants in Korea 1179

Table II. Sampling design for the analysis of antioxidants based on market share information.

Number of samples Number of samples Number of samples


from the upper from the middle from the lower
Food subcategory Number of samples 25% of market share 50% of market share 25% of market share
Soybean oil 12 6 4 2
Corn oil 12 6 4 2
Other vegetable oil 12 6 4 2
Shortening 12 6 4 2
Margarine 7 4 2 1
Seasoned dried fish 17 9 5 3
Dried fish 17 9 5 3
Salted fishery product 17 9 5 3
and frozen fishery
product (combined)
Chewing gum 7 4 2 1
Mayonnaise 10 5 3 2
Breakfast cereal 10 5 3 2
Total 133 69 41 23
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(figure 983.15, chapter 47, p. 4), and the Korean Analytical Method ( Japan Pharmacy Society 1995;
Food Code. (AOAC 1995; Japan Pharmacy Society KFDA 1999b). All samples and standards were run
1995; KFDA 1999b). in duplicate and the retention times were 5 min for
In the case of oil and fat, samples of 5 g were BHA, 4 min for BHT and 9 min for TBHQ. Mean
weighed (in case of lard or shortening, liquefied in recoveries of BHA, BHT and TBHQ were in the
bulk using 60 C water bath, and shaken to ensure ranges 81.8–89.2, 92.6–94.5 and 88.7–95.4%,
homogenecity) into separatory funnel (AOAC 1995). respectively. In case of oil and butter recovery and
Pentane (20 ml) was added in the funnel and CV% for BHA were 81.8% and 6.9, respectively, and
extracted with three 100-ml portions of saturated recovery and CV% for BHT were 94.5% and 3.5,
acetonitrile (saturated about 300 ml acetonitrile in respectively, and recovery and CV% for TBHQ were
separatory funnel by adding n-pentane until two 95.4% and 3.8, respectively. In the case of solid food
layers remain after shaking 2 min, and then removed recovery and CV% for BHA were 89.2% and 3.7,
and discarded n-pentane upper layer) (KFDA respectively, and recovery and CV% for BHT were
1999b). The acetonitrile layer was transferred to a 92.6% and 5.8, respectively, and recovery and CV%
round-bottom flask, and evaporated to 3–4 ml, using for TBHQ were 88.7% and 3.1, respectively. The
an evaporator with a water bath at <40 C, and detection limits for BHA, BHT and TBHQ were 3, 3
transferred to a 10-ml glass-stoppered graduated and 5 mg kg1, respectively.
cylinder. The flask was rinsed with small portion
non-saturated acetonitrile and rinses transferred to
Food consumption data
the cylinder until 10 ml was collected, then the rinses
evaporated to 1 ml using evaporator with a water Food consumption data for the assessment of daily
bath at <40 C (AOAC 1995). In case of solid food, intake of BHA, BHT and TBHQ were obtained from
samples of 5–40 g were weighed into a high-speed the Korea National Health and Nutrition Survey
blender, 100 ml pentane were added and the blender 1998 (KNHNS) (Ministry of Health and Welfare,
was swirled for 2 min. The pentane layer was 1999). The KNHNS was conducted based on the
transferred to round-bottom flask. The repeated National Health Promotion Act of 1995 (Ministry of
extractions were conducted twice with 100 ml Health and Welfare, 1995) by a research institute
pentane each time. The pentane extractions were experienced in nationwide surveys and the unique
evaporated to 20 ml. Pentane extractions were then nationwide nutrition survey in Korea. Briefly, the
transferred into the separatory funnel, and extracted survey visited 4828 households nationwide and
with three 100-ml portions of saturated acetonitrile. was completed for 2 months from November to
The next step was performed by the same methods December in 1998. The sample households were
for oil and fat described above (KFDA 1999b). selected by a stratified multistage sampling method
All samples were analysed by gas chromatography employing region and district as strata. Among those
(GC-FID; Hewlett Packard, Palo, Alto, CA, USA) 4828 households and 12 023 subjects visited, 4395
using the conditions shown in Table III. Gas households and 11 525 subjects agreed to participate.
chromatography was performed according to the The survey comprised different regions, age and
Korean Food Code and the Japanese Safety gender. Every 1 year and over in each sample
1180
H.-J. Suh et al.
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Table III. Consumption data of food in which the use of BHA, BHT and TBHQ is permitted in Korea in different region and age group (1998 KNHNS) (g/person day1).

Region and age (years): Total population Metropolitan Urban Rural 1–2 3–6 7–12 13–19 20–29 30–49 50–64 >65

Food categories Number of people 10 400 4011 2658 3731 288 721 911 1110 1419 3327 1650 974
Soybean oil 3.26 3.55 3.31 2.54 1.08 2.87 4.01 4.69 3.96 3.39 2.30 1.18
Corn oil 0.73 0.70 0.73 0.81 0.28 0.76 0.87 0.90 0.71 0.92 0.42 0.29
Other vegetable oil 0.17 0.10 0.24 0.22 0.06 0.12 0.08 0.15 0.27 0.17 0.13 0.28
Shortening 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00
Margarine 0.06 0.08 0.04 0.06 0.01 0.11 0.14 0.02 0.03 0.11 0.00 0.01
Seasoned dried fish 0.42 0.34 0.48 0.51 0.03 0.51 0.63 0.82 0.42 0.46 0.11 0.01
Dried fish 5.62 5.36 6.25 5.22 1.66 2.54 5.09 6.46 6.32 6.34 5.83 4.02
Salted fishery product 1.21 1.17 1.16 1.36 0.61 1.08 0.96 0.54 0.72 1.60 1.70 1.14
Frozen fishery product n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a.
Chewing gum 0.04 0.03 0.02 0.05 0.27 0.19 0.04 0.05 0.01 0.01 0.00 0.00
Mayonnaise 0.54 0.62 0.58 0.27 0.02 0.34 0.63 0.67 0.98 0.59 0.19 0.10
Breakfast cereal 0.73 0.97 0.68 0.24 1.32 4.45 1.87 0.65 0.41 0.25 0.00 0.14

KNHNS, Korea National Health and Nutrition Survey. n.a., Not available.
Estimated daily intakes of BHA, BHT and TBHQ antioxidants in Korea 1181

household was included in the survey. This survey the maximum permitted level (MPLi) of BHA, BHT
employed 1-day 24-h recall method to monitor and TBHQ in each food category and the mean food
individual dietary intake. Those who were unable intake data {F(ave)i} of total population.
to be interviewed individually such as children and EDIs1 and EDIs2 were adjusted with the standard
the elderly were interviewed with his/her guardian’s body weights (bwi) of the Recommended Dietary
help. To identify the types and quantity of food Allowances for Koreans in 2000 (Korean Nutrition
products used for cooking, the recipes for the foods Society 2000) for total population. This calculation
was surveyed by the interview of housewives or can be represented by the following expressions:
guardians. Also, the intake amounts of foods and
processed foods at eat-out as well as those in-house EDI1ðaveÞ i ¼ Cave FðaveÞ i
were surveyed through individual interviews. Food EDI1ð90thÞi ¼ Cave Fð90thÞi
intake of individuals was estimated using the recipes
EDI1ð95thÞi ¼ Cave Fð95thÞi
from each interviewed household and catering
services for schools, work sites, etc. EDI1ðaveÞ ¼ EDI1ðaveÞ i=bwi
The national survey methods and results, by EDI1ð90thÞ ¼ EDI1ð90thÞ i=bwi
region and by age, have been described in detail EDI1ð95thÞ ¼ EDI1ð95thÞ i=bwi
elsewhere (Ministry of Health and Welfare 1999;
EDI2i ¼ MPL i , FðaveÞi
Kim et al. 2003, 2004).
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EDI2ðaveÞ ¼ EDI2ðaveÞi =bwi : ð2Þ

Assessment of the estimated daily intakes (EDIs) of To evaluate the dietary intakes of BHA, BHT and
BHA, BHT and TBHQ TBHQ, EDIs1 and EDIs2 were compared with
ADI for BHA, BHT and TBHQ, evaluated by the
EDIs1 of BHA, BHT and TBHQ were calculated JECFA (Joint FAO/WHO Expert Committee on
based on individual food intake data and analytical Food Additives) as shown in Tables IV–VII (FAO/
data of 12 food categories (ten food categories for IPCS 1999).
TBHQ) for average and high consumers (90th and
95th percentiles of consumers only). For average
consumers, EDIs1(ave)i for each food category were Results and discussion
obtained by multiplying mean concentration (Cave)
Determination of antioxidants in foods
of BHA, BHT and TBHQ in each food category
and the mean food intake data {F(ave)i} of total The foods for which use of antioxidants is permitted
population. For high consumers, EDIs1(90th)i and are shown in Table I and were selected based on the
EDIs1(95th)i for each food category were obtained by Korea Food Additive Code for the analysis of BHA,
multiplying mean concentration (Cave) of BHA, BHT and TBHQ. Twelve food categories such as
BHT and TBHQ in each food category and 90th soybean oil, corn oil, other vegetable oil, shortening,
percentile intake data {F(90th)i} or 95th percentile margarine, seasoned dried fish, dried fish, salted
intake data {F(95th)i} of consumer only. The calcula- fishery product, frozen fishery product, chewing
tion method of EDIs1 of BHA, BHT and TBHQ was gum, mayonnaise and breakfast cereal were selected
similar to previous reports by Yoon et al. (2001, for BHA and BHT, and ten food categories
2003). EDIs2 of BHA, BHT and TBHQ, EDIs2(ave)i except mayonnaise, and breakfast cereal among
for each food category were calculated by multiplying those 12 food categories were selected for TBHQ

Table IV. Estimated daily intakes (EDIs1) of BHT and TBHQ based on analytical data and individual dietary intake data for average and
high consumers in Korea.

Daily intake (mg/person day1)

High consumers

Average consumers 90th percentile 95th percentile

BHT TBHQ BHT TBHQ BHT TBHQ


3 3
Chewing gum 0.7785 0.0657 0.3633 0.0307 0.3893 0.0329
Margarine 0.07743 – 0.0345 – 0.0523 –
Total
Daily intake 0.85593 0.06573 0.3978 0.0307 0.4416 0.0329
Daily intake (kg1 bw)* 0.01563 0.00123 0.0072 0.0006 0.0080 0.0006
ADI (%)** 0.0052 0.0002 2.4000 0.0857 2.6667 0.0857

*mg kg1 bw day1. **Comparison with ADI by the JECFA.


1182 H.-J. Suh et al.

Table V. Estimated daily intake (EDI2) of BHA based on the maximum permitted level and individual dietary intake data.

Maximum permitted Daily food intake for BHA daily intake


Food category level (mg kg1)1 average consumers (g/person)2 (mg/person)
Soybean oil 200 3.26 0.65
Corn oil 200 0.73 0.15
Other vegetable oil 200 0.17 0.03
Shortening 200 0.00 0.00
Margarine 200 0.06 0.01
Seasoned dried fish 200 0.42 0.08
Dried fish 200 5.62 1.12
Salted fishery product 200 1.21 0.24
Frozen fishery product 1000 n.a. –
Chewing gum 750 0.04 0.03
Mayonnaise 140 0.54 0.08
Breakfast cereal 50 0.73 0.04
Total
Daily intake 2.43
Daily intake (kg1 bw) 0.04
ADI (mg kg1 bw)3 0.5
ADI (%) 8.84
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1
Source: KFDA (1999a). 2Based on the ’98 Korea National Health and Nutrition Examination Survey, 1999. 3Based on the
JECFA. n.a., Not available.

Table VI. Estimated daily intake (EDI2) of BHT based on the maximum permitted level and individual dietary intake data.

Maximum permitted level Daily food intake for average BHT daily intake
Food category (mg kg1)1 consumers (g/person)2 (mg/person)
Soybean oil 200 3.26 0.65
Corn oil 200 0.73 0.15
Other vegetable oil 200 0.17 0.03
Shortening 200 0.00 0.00
Margarine 200 0.06 0.01
Seasoned dried fish 200 0.42 0.08
Dried fish 200 5.62 1.12
Salted fishery product 200 1.21 0.24
Frozen fishery product 1000 n.a. –
Chewing gum 750 0.04 0.03
Mayonnaise 60 0.54 0.03
Breakfast cereal 50 0.73 0.04
Total
Daily intake 2.38
Daily intake (kg1 bw) 0.04
ADI (mg kg1 bw)3 0.3
ADI (%) 14.42
1
Source: KFDA (1999a). 2Based on the ’98 Korea National Health and Nutrition Survey, 1999. 3Based on the JECFA. n.a.,
Not available.

(Table II). The total sample numbers for the analysis samples among ten food categories were analysed for
of BHA, BHT and TBHQ were calculated by TBHQ. BHA was not detected in any of those
Equation 1 takes into consideration as listed in samples. However, BHT was detected in margarine,
Table II. The Korea National Health and Nutrition and chewing gum among the 12 food categories.
Survey results of selected 12 food categories was In margarine, BHT was detected from only one
showed in Table III. sample among seven samples. The detected BHT
level was 9.05 mg kg1 BHT in chewing gum,
detected in three samples among the seven samples,
Estimated daily intake based on analytical data and
and the concentration of BHT ranged from not
individual dietary intake data (EDI1) of BHA, BHT
detected (n.d.) to 150.88 mg kg1. Therefore, the
and TBHQ
detection rate of BHT in margarine, and chewing
The 133 food samples among 12 food categories gum were 14.29, and 42.86%, respectively. The
were analysed for BHA, and BHT. A total 109 food mean concentration of BHT in margarine, and
Estimated daily intakes of BHA, BHT and TBHQ antioxidants in Korea 1183

Table VII. Estimated daily intake (EDI2) of TBHQ based on the maximum permitted level and individual dietary
intake data.

Maximum permitted level Daily food intake for average TBHQ daily intake
Food category (mg kg1)1 consumers (g/person)2 (mg/person)
Soybean oil 200 3.26 0.65
Corn oil 200 0.73 0.15
Other vegetable oil 200 0.17 0.03
Shortening 200 0.00 0.00
Margarine 200 0.06 0.01
Seasoned dried fish 200 0.42 0.08
Dried fish 200 5.62 1.12
Salted fishery Product 200 1.21 0.24
Frozen fishery product 1000 n.a. –
Chewing gum 750 0.04 0.03
Total
Daily intake 2.31
Daily intake (kg1 bw) 0.04
ADI (mg kg1 bw)3 0.7
ADI (%) 6.00
1
Source: KFDA (1999a). 2Based on the ’98 Korea National Health and Nutrition Survey, 1999. 3Based on the JECFA.
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n.a., Not available.

chewing gum were 1.29 and 25.95 mg kg1, respec- aspects, acute, short- and long-term toxicity,
tively. TBHQ was detected only in chewing gum carcinogenicity, and reproductive toxicity (EFSA
and not detected in the other nine food categories. 2004). In some studies, TBHQ was clastogenic in
The concentration of TBHQ in the chewing gum vitro and in vivo (Baunwart et al. 2001). But based on
presented 15.35 mg kg1 level in one sample among the data reviewed the Scientific Committee on Food
seven samples, and the mean concentration was (SCF) concluded that TBHQ is not carcinogenic
2.19 mg kg1. On the other hand, in Japan, the and that further genotoxicity studies are unnecessary
detection rate of BHA in instant noodles, animal fat, (EFSA 2004). Daily intakes of BHT and TBHQ
bread, biscuit among processed foods sold in 1983 based on analytical data and individual dietary data
was 12.0% and the rate of BHT in bread, biscuit and (EDI1) are shown in Table IV. For average
margarine was 10.4%. In 1995, the detection rate consumers, daily intakes of BHT and TBHQ were
of BHA was 12% in chewing gum, dried fishery 0.863 and 0.073 mg/person day1, respectively.
products and salted fishery products. The rate of The foods that contribute to the intakes of BHT
BHT was 2.3% in oils, dried fillet fishes and chewing and TBHQ were chewing gum and margarine. In
gum (Yoshio 1983, 1995). comparison with the ADI set by the JECFA, these
However, in comparison with Japanese study result were below 0.0052 and 0.0002%, respectively.
results, BHA, BHT and TBHQ have been hardly For 95th percentile consumers, daily intakes of
detected in foods for which use is permitted in BHT, and TBHQ as a portion of the ADI were
Korea, according to the results obtained from 2.67 and 0.09%, respectively. These results showed
previous studies as well as this study (Kim et al. that daily intakes (EDIs1) of BHA, BHT and TBHQ
1985, 1991). The reason might be that phenolic based on analytical data and individual dietary data
antioxidants such as BHA, BHT and TBHQ carry even among high consumers (95th percentile) in
toxicity and present a serious health hazard to Korea were remarkably below ADI as established by
humans, has been believed in Korea so BHA, BHT the JECFA.
and TBHQ have been little used in foods.
The toxicity of phenolic antioxidants has been
Estimated daily intake based on the maximum permitted
studied by many researchers. BHA has demonstrated
level and individual dietary intake data (EDI2 ) of BHA,
hyperplasia and hyperkeratosis in the forestomachs of
BHT and TBHQ
a variety of test animal species, but although benign
tumors were reported in the hamster forestomach, no Estimated daily intakes (EDIs2) of BHA, BHT and
carcinomas were induced in species other than rats. TBHQ based on the maximum permitted level and
BHT has been reported as showing evidence that it individual dietary intake data are shown in Tables V–
may act as a promoting agent for some types of VII. The EDIs2 of BHA, BHT and TBHQ were
chemical carcinogenesis in test animals. But in both 2.43, 2.38 and 2.31 mg/person day1, respectively.
antioxidants, the relevance of these effects to humans In comparison with the ADIs set by the JECFA,
is unclear (Sherwin 1990). The toxicity of TBHQ these results were 8.84, 14.42 and 6.00%, respec-
has been extensively studied, including toxicokinetic tively. Overall, EDIs2 of BHA, BHT and TBHQ
1184
H.-J. Suh et al.
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Table VIII. Estimated daily intake of BHA in several countries.

Australia and
Korea1 Korea2 China3 Spain4 France5 Spain6 Japan7 New Zealand8 USA9 Brazil9

EDI ADI EDI ADI EDI ADI EDI ADI EDI ADI EDI ADI EDI ADI EDI ADI EDI ADI EDI ADI
Country (mg kg1 bw) (%) (mg kg1 bw) (%) (mg kg1 bw) (%) (mg kg1 bw) (%) (mg kg1 bw) (%) (mg kg1 bw) (%) (mg kg1 bw) (%) (mg kg1 bw) (%) (mg kg1 bw) (%) (mg kg1 bw) (%)
Average 0.00 0.00 0.04 8.84 0.005 1 0.48 96 0.02 4 0.25 50 0.003 0.6 0.39 78 0.4 80 0.09, 0.15 18, 30
consumption
1
Based on individual dietary data and analytical data (present study). 2Based on individual dietary data and the maximum permitted level specified in national food standards (present study). 3Based on
poundage data (WHO 2000). 4Based on poundage data (WHO 2000). 5Based on household economic survey or retail sales surveys (WHO 2000). 6Based on household economic survey or retail sales
surveys (WHO 2000). 7Based on individual dietary records and analytical data by market basket survey (WHO 2000). 8Based on individual dietary records and maximum levels specified in national
food standards (WHO 2000). 9Based on model diet and national maximum limits (WHO 2000). 10Based on survey on household budgets (IBGE) and market survey (Datamark) and the maximum
permitted level (Baunwart et al. 2001).
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Estimated daily intakes of BHA, BHT and TBHQ antioxidants in Korea


Table IX. Estimated daily intake of BHT in several countries.

Korea1 Korea2 USA3 Japan4 Brazil5

EDI ADI EDI ADI EDI ADI EDI ADI EDI ADI
Country (mg kg1 bw) (%) (mg kg1 bw) (%) (mg kg1 bw) (%) (mg kg1 bw) (%) (mg kg1 bw) (%)
Average consumption 0.01563 0.0052 0.04 14.42 0.39 130 0.00085 0.028 0.05, 0.1 16.67, 33.3
1
Based on individual dietary data and analytical data (present study). Based on individual dietary data and the maximum permitted level specified in national food standards (present study). 3Based on
2

model diet and national maximum limits (WHO 2000). 4Based on individual dietary records and analytical data by market basket survey (WHO 2000). 5Based on survey on household budgets (IBGE)
and market survey (Datamark) and the maximum permitted level (Baunwart et al. 2001).

1185
1186
H.-J. Suh et al.
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Table X. Estimated daily intake of TBHQ in several countries.

Korea1 Korea2 China3 China4 USA5 USA6 Brazil7

EDI ADI EDI ADI EDI ADI EDI ADI EDI ADI EDI ADI EDI ADI
Country (mg kg1 bw) (%) (mg kg1 bw) (%) (mg kg1 bw) (%) (mg kg1 bw) (%) (mg kg1 bw) (%) (mg kg1 bw) (%) (mg kg1 bw) (%)
Average consumption 0.00123 0.0002 0.04 6.0 0.004 0.6 0.69 100 0.14 20 0.37 50 0.07, 0.12 10, 17
1 2 3
Based on individual dietary data and analytical data (present study). Based on individual dietary data and the maximum permitted level specified in national food standards (present study). Based on
poundage data (WHO 2000). 4Based on individual dietary records (WHO 2000). 5Based on poundage data (WHO 2000). 6Based on model diet (WHO 2000). 7Based on survey on household budgets
(IBGE) and market survey (Datamark) and the maximum permitted level (Baunwart et al. 2001).
Estimated daily intakes of BHA, BHT and TBHQ antioxidants in Korea 1187

based on the maximum permitted level and indivi- margarine; and TBHQ was detected only from
dual dietary intake data as well as EDIs1 of BHA, chewing gum. The EDIs1 of BHA, BHT and
BHT and TBHQ based on analytical data and TBHQ based on analytical data and individual
individual dietary data were relatively lower than dietary intake data even among high consumers
ADI set by the JECFA. (95th percentile) in Korea were below the ADI
In addition, EDIs of BHA, BHT and TBHQ as established by the JECFA. The EDIs2 of BHA,
according to this paper were significantly lower than BHT and TBHQ based on the maximum permitted
the theoretical maximum daily intakes (TMDI) by level and individual dietary intake data were remark-
the Budget method (Yoon et al. 1991). Because the ably below the ADI by the JECFA. The reasons
Budget method is used for risk assessment to might be that Korean food manufacturers do not use
minimize the cost and tends to overestimate the the antioxidants excessively, and food consump-
daily intakes of food additives. tion of the selected food categories in Korea is
relatively low.
In our study, the current pattern of use of
Comparison with other countries antioxidants by the food industry was not consid-
ered. Further research considering the launch of
In comparison with other countries, estimated daily new products and the use of different formulations
intakes (EDIs1) of BHA, BHT and TBHQ based on by the industry based on refined dietary intake
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analytical data and individual dietary intake data for data are needed to obtain habitual intakes of
average consumers in Korea were remarkably lower phenolic antioxidants for future risk assessment in
than EDIs of other countries (Tables VIII–X). Korea.
Although there was a variation in the measuring
methodology, the intake levels of BHA, BHT and
TBHQ among ten member countries (six member Acknowledgements
countries for TBHQ) of CODEX were 0.003–0.48,
0.00085–0.39 and 0.004–0.69 mg kg1 bw, respec- The paper was the part of the project Daily Intake
tively, based on the WHO (2000) report. Among Estimate for Food Additives in Korea, which was
those countries, Japan has the lowest intake levels on supported by the Health Technology Planning and
the BHA and BHT. In the present study, however, Evaluation Board, Ministry of Health and Welfare
the EDIs1 of BHA, and BHT based on analytical in Korea.
data and individual dietary intake data in Korea
were 0 and 0.01563 mg kg1 bw, which were even
lower than those of average consumers in Japan. The References
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