I NTAKE C ALCULATIONS OF P ESTICIDE R ESIDUES In this section, intake calculations or dietary exposure from different parts of the

11.3.2 I NTAKE C ALCULATIONS OF P ESTICIDE R ESIDUES In this section, intake calculations or dietary exposure from different parts of the

world using different approaches are presented.

310 Analysis of Pesticides in Food and Environmental Samples

11.3.2.1 Deterministic Approach The results from the EU-coordinated monitoring program are used to calculate both

the chronic and acute intake every year. 16 For the chronic intake, the 90th percentiles of all the results was used as concentration giving a worst-case situation. Consump- tion figures were taken from the WHO Standard European Diet, using 60 kg as body weight. The exposure remains well below the ADI for all combinations of pesticide and commodity, ranging from 0.009% of ADI for fenhexamid in strawberry to 5.36% of the ADI for the dithiocarbamates in lettuce. For the acute intake, the data for the high or acute consumption from UK were used and the calculation was performed with the highest residue found. For eight pesticides (deltamethrin, dimethoate, lambda-cyhalothrin, dithiocarbamates, methamidophos, methidation, methomyl, and oxydemeton-methyl), this gave results exceeding the ARfD. The highest intake was 47 times the ARfD for oxydemeton-methyl in apples.

Using different figures for the residue contents, for example, MRLs or data from monitoring programs can have a great impact on the intake, which are shown by an example from a Korean intake estimate. 89 Data for consumption was from a 1998,

Nation Nutrition Survey and data for residue levels were found analyzing 6164 samples representing 107 different kinds of food commodities. All the samples were collected at the same commercial market in 2001. Using MRLs as residues caused that for 16% of the analyzed pesticides the intake exceeded the ADIs (Codex values). When residue levels from the analyzed samples were used, the intake decreased dramatically to <0.15% of ADI.

For some studies, the pesticide intakes are limited to include the OCPs that bioaccumulate. From Uzbekistan, estimated monthly intake for the different isomers of HCH were 1

90 on food type. –60 mg=month for a-HCH; 2–140 mg=month for b-HCH depending The samples used for analyses were collected from three towns in February 2001. Twelve different food types were collected among them: animal

products, fish, oils, vegetables, and cereals. The consumption data were collected in one city and comprised of 101 households. Information was gathered about the food consumption in the previous month.

11.3.2.2 Total Diet and Duplicate Diet Studies In India, during 1999 –2002, a kind of duplicate diet study was performed for

men aged 19 91 –24 years. Every month vegetarian and nonvegetarian total diet samples comprising breakfast, lunch, and dinner were collected. Lindane was the pesticide most widely found, but the frequency decreased throughout the study from about 90% in 1999 to about 25% in 2002. The Codex ADI for lindane of 0.008 mg=kg body weight was exceeded in 1999 for the vegetarian diet and in 1999 and 2000 for the nonvegetarian diet. An explanation for the high contribution from lindane could be that about 21% of the consumption in the study came from milk and milk products, which another study showed could be highly contaminated with lindane.

In Kuwait, the dietary exposure to organophosphate pesticides was determined in the total diet and the food consumption survey was conducted as a 24 h dietary recall

Levels of Pesticides in Food and Food Safety Aspects 311 study. 92 The 6700 participants were interviewed about what they had consumed

the previous day. All together 140 food items, divided into 11 food categories, were selected to represent the list of the Kuwaiti total diet study. The Kuwaiti diet is characterized by a high intake of cereals (grain), vegetables, and fruits and >90% of the food is imported. Intakes for 19 different age groups were calculated and all amounted to <6% of the ADIs. For males 15 –19 years, diazinon contributed most to the intake. Grain and vegetables were the food groups that contributed most to the intake.

In the period 1986

The consumption data were based on two nationwide surveys covering about 50,000 –1991, the US FDA has performed a Total Diet Study. participants. In the studies, over 5000 types of foods were identified but to the

Total Diet Study 234 foods were selected to represent all 5000 foods. The dietary intakes of pesticide residues were estimated for eight age=sex groups. In Table 11.8, the daily intakes per kilogram body weight for males 14 –16 years are compared with the relevant ADI (Codex values). The six pesticides that contributed most to the daily intake and the pesticides that contribute most to the ADI are shown. The overall conclusion was that the intakes of pesticides are well below the ADI for all age groups.

11.3.2.3 Cumulative Exposure EPA has performed cumulative risk assessment for four groups of pesticides 94

namely organophosphates, N-methylcarbamates, triazines, and chloroacetanilides. In these assessments, not only the dietary exposure is calculated but also the exposure from water and residential uses. For triazines, exposure through food was not considered as relevant and for chloroacetanilides only two pesticides were included so these assessments are not summarized.

TABLE 11.8 Six Pesticides That Contribute Most to the Intake (mg=kg bw) and ADI (%)

for Males 14–16 Years in the U.S. Total Diet Study a

Pesticides That Pesticides Contribute Most

That Contribute to the Intake

Most to the ADI % of ADI Chlorpropham (no ADI given)

Intake mg=kg bw

Dieldrin 3 Thiabendazole

Heptachlor 1 Malathion

Omethoate 0.53 Dichloran, total

Malathion 0.48 Permethrin, total

Dicofol (sum) 0.40 Carbaryl

Carbaryl 0.31 a Values taken from the published paper.

312 Analysis of Pesticides in Food and Environmental Samples

TABLE 11.9 Exposure and MOE at the 99.9th Percentiles for Children 1–2 Years and Children 3–5 Years Which Have the Lowest MOEs as Well as for Adults 20–49 Years

(mg=kg bw) MOE Children 1 –2 years

(mg=kg bw)

MOE

2.6 30 3.8 37 Children 3 –5 years

2.3 34 3.7 42 Adults 20 –49 years

For both organophosphates and the carbamates, residue data were primarily obtained from the USDA PDP program collected from 1993 to 2003 or from 1993 to 2004. The consumption data are from the USDA’s Continuing Survey of Food Intakes by Individuals, 1994 –1996=1998. In this survey, ca. 21,000 participants were interviewed over two discontinuous days. Processing factors are included in the estimates; undetectable residues were set to zero.

In the study, the MOE approach as well as the probabilistic approach was used. For the organophosphates, the IC was methamidophos, whereas for the carbamates oxamyl was chosen as IC (Table 11.9).

The foods that contributed most to the children’s (1 –2 year) exposure to carba- mates were strawberry and potato, whereas the pesticides that contributed most were methomyl and aldicarb. For organophosphates, the foods that contributed most to the intake for children of 3 –5 years were snap bean and the pesticides that contributed most were methamidophos and phorate.

In a study from Brazil, 95 the TEF as well as the probabilistic approach were used. In this study, methamidophos and acephate were used as index compounds.

TABLE 11.10 Cumulative Intake (mg=kg bw=day) of Choline Esterase Inhibitors at the 99.9% and 99.99% Percentile

Brazil

Total Population ARfD

Children (0–6 Years)

99.9% 99.99% (mg=kg bw)

Percentile Percentile Methamidophos

35.1 134 Source: From Caldas, E.D., Boon, P.E., and Tressou, J., Toxicology, 222, 132, 2006.

Levels of Pesticides in Food and Food Safety Aspects 313

TABLE 11.11 Cumulative Intakes of Choline Esterase Inhibitors for the Adults and Children in Denmark Using Methamidophos and Chlorpyrifos as Index Compounds

Chlorpyrifos Methamidophos Equivalents, Equivalents, TEF NL

TEF United States 0 LOD

0 LOD ½ LOD ½ LOD Adult

Child Adult Child Fruits, Vegetables, and Cereals

0.0029 0.4200 1.0800 intake m g=kg bw=day

% of 0.8 2 2 5 0.03 0.07 11 27 ADI

Source: From Jensen, A.F., Petersen, A., and Granby K., Food Addit. Contam., 20, 776, 2003. With permission.

The food consumption data used in this study were obtained from the Brazilian Household Budget Survey, 2002 –2003. Data were collected from 45,348 households corresponding to 174,378 individuals. Each household recorded the amount of food entering in a diary over seven consecutive days and this was considered as eaten. For each individual, the week consumption was decomposed into daily consumption patterns over 7 days. Residue data were obtained from the Brazilian national program on pesticide residues. A total of 4001 samples of tomato, potato, carrot, lettuce, orange, apple, banana, papaya, and strawberry were analyzed for their contents of pesticides. Samples with nondetectable levels were assigned a value of ½ LOQ for the index compound. Processing factors were included. In Table 11.10, the intake at the 99.9% and 99.99% percentile for both index compounds are shown. Tomato was independent of IC definitely, the crop that contributed most to the total intake (>65%).

Cumulative risk assessment has been made for the Danish population for the chronic intake. 96 Residue data were from the Danish monitoring program

1996 –2001, whereas the consumption data were from the Danish nationwide food consumption survey in 1995. Average values were used for residue levels. Two different IC compounds were used namely chlorpyrifos and methamidophos. The TEF values were taken, respectively, from a Dutch paper and the US EPA. Process- ing factors were included in the calculations. The intake was calculated both with nondetectable residues as zero and as ½ LOD. This affected not only the intake (Table 11.11) but also the pesticides or commodities that contributed most to the intake (Figure 11.4).

314 Analysis of Pesticides in Food and Environmental Samples

Rest 48 commodities

Rest 48

17% commodities

Wheat Cucumber

5% Potato Cauliflower

Apple 14% Grape

Rest 33 Rest 33 pesticides Chlorfenvinphos

Diazinon methyl 12%

14% Methamidophos Methamidophos 25%

FIGURE 11.4 Commodities (two upper diagrams) or pesticides (two lower diagrams) that contributed most to the cumulative intake for the Danish population of choline esterase inhibitors in chlorpyrifos equivalents. To the left: nondetectable ¼ 0; to the right: non- detectable ¼ ½ LOD. (From Jensen, A.F., Petersen, A., and Granby K., Food Addit. Contam.,

20, 776, 2003. With permission.)