1 23 Environmental Monitoring and Assessment An International Journal Devoted to Progress in the Use of Monitoring Data in Assessing Environmental Risks to Man and the Environment ISSN 0167-6369 Volume 186 Number 1 Environ Monit Assess (2014) 186:217-228 DOI 10.1007/s10661-013-3367-0 Assessment of dietary intakes of nineteen pesticide residues among five socioeconomic sections of Hyderabad—a total diet study approach Agatha Betsy, Sudershan Rao Vemula, SN Sinha, Vishnu Vardhana Rao Mendu & Kalpagam Polasa
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Environmental Monitoring andAssessmentAn International Journal Devoted toProgress in the Use of Monitoring Datain Assessing Environmental Risks toMan and the Environment ISSN 0167-6369Volume 186Number 1 Environ Monit Assess (2014)186:217-228DOI 10.1007/s10661-013-3367-0
Assessment of dietary intakes of nineteenpesticide residues among five socioeconomicsections of Hyderabad—a total diet studyapproach
Assessment of dietary intakes of nineteen pesticide residuesamong five socioeconomic sections of Hyderabad—a total dietstudy approach
Agatha Betsy & Sudershan Rao Vemula & SN Sinha &
Vishnu Vardhana Rao Mendu & Kalpagam Polasa
Received: 27 March 2013 /Accepted: 24 July 2013 /Published online: 31 August 2013# Springer Science+Business Media Dordrecht 2013
Abstract Total diet study approach was used to assessthe dietary intakes of pesticide residues among the selectpopulation in Hyderabad. When assessed by a food fre-quency questionnaire, it was found that the food intakesvaried among five socioeconomic sections (SES).Therefore, we intended to compare the intakes of pesticideresidues through these foods among the five SES. A totalof 195 foods from different markets were collected andanalyzed for 19 pesticides. The residues were analyzedwith a gas chromatograph and were confirmed with massspectrometry. About 51 % of the samples were detectedwith one or more residues. Thirteen out of the 19 residueswere present in levels above detection limits in variousconcentrations. The median concentrations of the residuesin all the samples tested, ranged from 0.00010 to0.33 mg/kg. Highest median concentration was for β-HCH in water samples. Exposures to all the residues werebelow the respective ADIs at both mean and 95th percen-tile levels of food intakes with highest estimated dietaryintakes (EDIs) of β-HCH in both the cases. The EDIs ofβ-HCH were the highest among all the residues at boththe intake levels among all the SES. The EDIs of β-HCHwere significantly higher in lower SES than higher SES
possibly due to the consumption of rice cooked in watercontaminated with β-HCH. EDIs for other residues didnot differ significantly among the five SES.
Around 234 pesticides are registered for use in agri-culture in India against various pests and diseases(Singh and Battu 2008). Pesticides mainly function asinsecticides (used against insect pests), herbicides (forkilling and controlling weeds), fungicides (against dis-eases), rodenticides, and others. They are classified onthe basis of their chemical composition as organophos-phate compounds, organochlorines, synthetic pyre-throids, carbamates, bio-pesticides, etc. (CSA, 2007).
Several studies in India have shown persistent occur-rence of various organochlorine pesticides (OCPs) likehexachloro-cyclohexane (HCH), dichloro-diethyl-trichloroethane (DDT), aldrin, and dieldrin in differentfoods and drinking water samples from different parts ofIndia (Battu et al. 1989; Dikshith et al. 1990; Gupta et al.1982; Kang et al. 2000; Kannan et al. 1992; Kaphaliaet al. 1990; Kole et al. 2002; Kumari et al. 2002; Noronhaet al. 1980; Singh, 2002; Shukla et al. 2006). HCHisomers (1,2,3,4,5,6-hexachlorocyclohexane) and DDTmetabolites [1,1,1-trichloro-2,2 bis (p′ chlorophenyl eth-ane)] are being used in India for a long time due to theirlow cost and versatile action against various pests
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A. Betsy : S. R. Vemula (*) : S. Sinha :K. PolasaFood and Drug Toxicology Research Centre (FDTRC),National Institute of Nutrition (NIN-ICMR),Hyderabad 500007 Andhra Pradesh, Indiae-mail: [email protected]
V. V. R. MenduDivision of Bioinformatics and Biostatistics, NationalInstitute of Nutrition (NIN-ICMR),Hyderabad, Andhra Pradesh, India
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(Kannan et al. 1992). OCPs, being lipophillic in nature,have a tendency to accumulate in fatty tissues as adiposetissues of animals and milk of humans and bovine. Highlevels of HCH (6,200 ng/g) and DDT (1,200 ng/g) weredetected from human milk samples collected from south-ern India (Tanabe et al. 1990). However, levels of HCHand DDTs were shown to continuously decrease in thebovine milk samples from India (Dethe et al. 1995;Mukherjee and Gopal 1993; Pandit et al. 2002).
The use of these highly persistent OCPs has lead totheir sustained presence in trace amounts in soil, waterand air leading to their entrance into the food chain. Inrecent studies, the levels of DDT (and its metabolites )and HCH (and its isomers) were detected below MRLsin most of the wheat flour (Toteja et al. 2003) and rice(Toteja et al. 2006) samples, and the dietary exposuresdue to these foods were in minute proportions as com-pared to ADIs by FAO (FAO, 1986). Although, someof the samples were found to have levels above theMRLs. The authors suggested that they could be due toaccidental contact with the chemical. The presence ofthese chemicals in the staple crops was supposed to bedue to their ubiquitous presence in the environment.
Vegetable samples collected at harvest from farmer’sfields around the districts of Hyderabad and Guntur inthe south Indian state of Andhra Pradesh, recorded HCHresidues above MRL (0.25 ppm) while residues of DDTand cypermethrin were found to be belowMRL (3.5 and0.2 ppm, respectively; CSA 2007). Similarly, yet anoth-er study in the Srikakulam district of the same state alsoshowed residues of HCH, DDT, aldrin (including diel-drin), endosulfan, and methyl parathion in vegetables,below the MRLs (Reddy et al. 1998).
Considering the results of studies from AndhraPradesh and other states and due to lack of recent studieson samples analyzed from southern India for dietaryexposures through the diet as whole and not singlefoods, the present study was undertaken with an objec-tive to check the presence of nineteen pesticides resi-dues, already reported to be present in the foods, andassess their exposures through total diet study approach.
Materials and methods
Study design
Hyderabad is the capital of Andhra Pradesh with apopulation of 6,809,970 (2011 census). The city of
Hyderabad is situated on the Deccan plateau at analtitude of 1,778 ft and occupying an area of650 km2. Predominant topography of the city is slop-ing, rocky terrain, and paddy is the major crop grownin surrounding fields. It is divided into 15 circlesconsisting of 5 SES.
Food consumption data for 5 SES of Hyderabadwere obtained. Information about most commonlyconsumed foods and their markets of purchase wascollected by a food frequency interview schedule(FFIS). Selected foods were purchased from the re-spective markets and were processed as table ready inlaboratory and analyzed for select pesticides. The con-sumption data and the pesticide concentration datawere combined to calculate the exposure estimates.The estimates were then compared with the referencetoxicological values.
Study population
Population of Hyderabad was divided into 5 SESaccording to HUDA (Hyderabad Urban DevelopmentAuthority) classification. A total of 157 householdswere selected from all the SES and administered avalidated food frequency interview schedule (FFIS).The SES were selected by cluster random samplingand households in each SES were selected by system-atic random sampling.
Selection of foods
Twenty most commonly consumed foods and watersamples were selected for analyzed. Along with them,only the foods which were reported to be detected withthe select pesticides and the foods for which no infor-mation was available were also selected for analyses.The recently conducted Andhra Pradesh Total DietStudy (APTDS 2010) also provided us with in-formation about the foods already been detectedwith these select residues. The foods included foranalyses were rice, wheat flour, red gram (dhal),tomato, lady’s finger, spinach, amaranth, potato,green chili, milk, mango, fish, and fowl. Drinkingwater samples which were used for cooking thefoods were also collected to calculate the totalconcentration due to the raw food and the waterused for cooking it.
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Collection of food samples
Foods were purchased from 13 markets that essentiallycater to 5 SES. Food samples representing HIG werecollected from supermarkets, those for MIG were pro-cured from retail shops and those representing LIGwere collected from rythu bazaar (a market place wherefarmers directly sell their produce to the consumers).About 1.5 to 2 kg of each food item was collected (toobtain a final edible portion of one kilogram) in sterilezip-lock pouches (for rice, wheat flour, red gram(dhal), tomatoes, lady’s finger, potatoes, fowl, fish,mangoes, and green chilies), sterile jute sacs (for spin-ach and amaranth, as they were spoiled in zip-lockpouches), and sterile amber glass bottles (for milkand water). Perishable foods such as fowl, fish, water,and milk were transported in ice packing, and otherfoods were transported at ambient temperature.
Processing of the foods
Edible portions of the foods were processed accordingto local household practices in table ready form includ-ing picking, sieving, washing and cooking. De-ionizedwater was used for cooking, wherever required.Stainless steel vessels like containers, ladles, covers,spoons, trays, and PTFE chopping boards were usedfor cooking. No chemical detergent was used for wash-ing to avoid external contamination, and vessels werethoroughly washed with hot water and dried in ovenbefore re-use to prevent cross contamination. Thefoods were weighed before and after cooking. Theamount of water added, temperature, and time requiredfor cooking were already standardized during AP-TDS, and the same conditions were followed for thepresent study. The cooked foods were cooled, homog-enized, and stored in PTFE containers at −20 °C tillanalyzed. Samples were procured and processed fromOctober 2010 to May 2011.
Selection of pesticides
Nineteen residues were analyzed including one organ-ophosphate compound (chloropyriphos), one syntheticpyrethroid (total cypermethrin), and 17 organochlorineresidues and their derivatives. The isomers of HCH; α,β, γ, and δ have different physico-chemical character-istics and toxicity profiles (Herbst 1982). Therefore,they were considered as individual contaminant
residues. Selection of pesticides in AP-TDS (2010)was based on several earlier reports from India (AP-TDS, 2010; Battu et al. 1989; Dikshith et al. 1989;Kumari et al. 2003; Pandit et al. 2002; Toteja et al.2003; Toteja et al. 2006). The use of chlordane, aldrin,dieldrin, and DDT was banned or restricted in Indiasince long during 1960s, but they were included foranalysis due to their probable lipophilicity, long-termpersistent nature, and lower ADIs. Chlorpyriphos, en-dosulfan and its derivatives, and cypermethrin are stillamong the most used pesticides in India (Directorate ofPlant Protection et al. 2010).
Analyses of the samples
Extraction of pesticide residues
The cooked wet samples were extracted with acetonitrile(MeCN with 1 % glacial acetic acid) as 1 mL/g(Anastassiades and Lehotey 2003). Fish and fowl sam-ples were additionally cleaned up with C-18. Graphitizedcarbon black was also tested for cleaning of these sam-ples, but a lower recovery was obtained. All the glass-ware in contact with the samples were soaked overnightin 1M HNO3 and washed. Glassware was rinsed withpure acetone before use.
Quantification of pesticide residues
Gas chromatograph (Varian 3800) equipped with elec-tron capture detector (GC-ECD) was used for quanti-fication. The oven temperature of GCwas at 100 °C for2 min, programmed from 100 °C to 190 °C at 5 °C permin held for 5 min, and maintained at 250 °C for 4 min.The total run time was 35 min and 1 μL was injectedfor quantification and confirmation. The detector andinjector port temperatures were 300 °C and 270 °C,respectively. A 5 % phenyl 95 % methyl polysiloxonecolumn was used with internal diameter of 0.53 mm,thickness of 0.50 mm, and with 30 m length with splitless system. Carrier gas used was Iolar-1 nitrogen(99.999 % purity) and the flow rate was 1.5 mL/min.
GC-MS/MS conditions
GC-MS/MS (Varian Saturn 2200) was used for confir-mation of the samples. Mass spectra were recorded inscan mode swith a mass range of 40–500 amu at a scanrate of 1 s/scan. The emission current of the ionization
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filament was set to 10-lA, which generated electrons at70 eV of energy. The transfer line, trap, and manifoldtemperature were set at 270 °C, 170 °C, and 40 °C,respectively (Sinha et al. 2011).
Recovery studies
Recoveries were calculated to check the efficacy of theextraction and were between the limits of 70–120% forall the non animal food matrices. The percentage ofrecovery of each pesticide was calculated by compar-ing the peak area ratio of the spiked standards withthose of the pure standards. However, spinach andamaranth showed the lowest mean recoveries (72 %and 75 %, respectively). The recoveries of fish andfowl samples were 67 % and 61 %, respectively.Calibration curves were constructed using 6 differentconcentrations of spiked pesticides (250, 100, 75, 50,10, and 5 ng/g in each food matrix) and plotted againstthe area counts. At least 5 repeat determinations wereperformed for each concentration on the calibrationcurve . Cal ibra t ion s tandard concent ra t ionsencompassed the entire linear range of the analysis.The limit of determination (R2) of 0.9932 was obtainedfor spiked concentration of all 19 pesticide residuesstandards on GC (ECD).
Limits of detection (LOD)
LOD was determined at a fortification concentrationwhen the signal-to-noise ratio was 3:1 for each pesti-cide. The lowest LOD of instrument was obtained as0.1 ng/g. Lowest limit of method validation (LLMV)was 0.186 ng/g for γ-HCH. The LOD for fortifiedsamples ranged from 1 ng/g for γ-HCH in tomato to5 ng/g for cypermethrin in spinach samples. The LODand LOQ were determined on the basis of 1:3 and 1:10noise-to-signal ratio with minimum possible interfer-ences from the co-extractives.
Calculation of the concentrations was done usingthe following formulae:
IRF ¼ Area IS � Conc:SCð Þ.
Conc:IS � Area SCð Þ
Where,
IRF is the internal response factor of the GC (ECD)IS is the internal standardSC is the sample analyte
Concentration of SC.g of sample
¼ Conc:IS � area counts of SC � IRFð Þ.area counts IS
The samples were confirmed with GC MS/MS(Varian) and were quantified. The area ratio of primaryand secondary ions in the MS had to be within 20 % ofthe theoretical value.
Quality control/quality assurance
Pure standards of individual pesticides were injected toconfirm the retention time (RTs), which were matchedwith those present in samples within ±3 s. One samplefrom each set of 13 samples was fortified with themixture of the analytes standard (100 ng/g) and wasextracted and run with other samples. Laboratory re-agent blanks were treated as actual samples and wererun with the set, and the blank value was subtractedfrom the sample values.
Assessment of dietary intakes
Estimated daily intakes (EDIs) were calculated bycombining the consumption data and the concentrationdata. It was necessary for calculation that the concen-trations below detectable limits (BDL) are assigned anumeric value. Concentration of the samples BDL wastaken as LOD providing the upper bound (UB) esti-mates as recommended internationally (WHO 2005).Trace concentrations between the LOD and LOQ wereassigned a value equal to half of the LOQ.
Median concentrations were obtained for dietaryintake assessments by pooling all the foods from dif-ferent markets. The median levels of concentrationsprovide a more realistic and appropriate estimation oflong term exposures to residues which are comparedwith the ADIs, which are lifetime toxicological refer-ences (FAO, 1997). Intakes of residues were calculatedby multiplying the median concentrations of residueswith the consumption data obtained by the FFIS.Exposure estimates were calculated at mean and 95thpercentile levels of food consumptions to obtain thenormal and worst case scenario, respectively. The es-timated intakes for average weight of adult populationin India (50 kg) were finally reported as mg/kg bw/dayand were compared with the respective ADIs.
Estimated Daily Intakes =∑ (pesticides averageconcentration in a food (mg/kg)×daily consumption
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of the food (g/day/person)/50 kg (average weight ofadult population
Statistical analyses
Food intakes were calculated at mean and 95th percen-tile levels and the concentrations of pesticides in foodswere calculated at 25th percentile, median, and 75thpercentile. Differences in the food consumptionsamong various SES were tested by analyses of vari-ance (ANOVA) with post hoc comparison by leastsignificance difference (LSD). The median residueconcentrations were compared with the MRL valuesgiven by Food Safety and Standards Authority of India(FSSAI, 2011).
Results
Food consumption
Food consumption data were obtained by a validatedFFIS for the 5 SES. Cooked rice was consumed inhighest quantities among all the foods in 5 SES.There were differences in the eating habits among thefive SES in terms of quantities of foods consumed.Cooked rice was consumed more in lower SES, whilefruits and vegetables were consumed in higheramounts by HIG and MIG. Food consumption at meanand 95th percentile intake levels is shown in Tables 1and 2.
Concentrations of pesticides
Nineteen pesticide residues were analyzed in 12 foodsand drinking water samples collected from 13 places inthe city. Over a half (51 %) of the samples weredetected with various concentrations of 13 pesticides.Concentrations of aldrin, dieldrin, β-endosulfan, endo-sulfan sulfate, and chlordane isomers (α and γ) werenot above the detection limits in any of the testedsamples from any of the markets. None of the mangoand fowl samples were detected with any pesticideresidue. Heptachlor was detected only in 4 samples oflady’s finger. Tomato and spinach samples were de-tected with maximum number of residues, and fishsamples were detected with only the residues of β-HCH, though all the levels were below the MRLs byFSSAI (2011).
The highest median concentration of residues insamples was of β-HCH (0.33 mg/L) in water samplesfollowed by levels of cypermethrin in red gram (dhal)and green chillies (0.293 mg/kg).
Median concentration of β-HCH in milk samples(0.049 mg/L) also was higher than the FSSAI limits of0.02mg/L.
The HCH and DDT isomers, wherever detected,except in wheat flour samples, were many folds belowtheir respective MRLs. There are no statutory limits forDDT in cereals grains in India. However, the ricesamples were detected with trace presence of o′p′DDE, o′p′ DDD, and p′p′ DDT. Trace residues oflindane and o′p′DDE were also detected in wheat floursamples exceeding the MRL of zero in milled cerealgrains.
Alpha endosulfan was only detected in red gram(dhal) and green chilies samples. Median concen-trations of residues in all the tested foods aregiven in Table 3.
Dietary exposure assessment
Estimated daily intakes (EDIs) were calculated foreach of the pesticide residues in all the SES. Intakeswere estimated at upper bound concentration levels(i.e., the values BDL were given a numeric value ofLOD) and both mean and upper bound (95th percen-tile) levels for food intake. The estimated dietary in-takes of none of the pesticide residues exceeded theADIs at mean and 95th percentile levels of food in-takes. The EDIs for β-HCH were highest among all theresidues in all the 5 SES. The highest EDI of β-HCHwas found in LIG (22.24 μg/kg bw/day, 44.4 % ofADI) at mean levels and in SD (40.2 μg/kg bw/day,80.4 % of ADI). The EDIs were highest for β-HCH inSD at 95th percentile intake levels, due to muchhigher intakes of cooked rice than in other SES.The exposure estimates for β-HCH were signifi-cantly higher in lower SES (LIG, IL, SD) than inMIG and HIG at both the levels of food intakes.However, there were no significant differences inthe EDIs of other residues among various SES.The EDIs for aldrin were lesser than other residues butpercentage of ADIs were higher than many other resi-dues due to its lower ADI (Tables 4 and 5). The contri-butions of various foods to total EDI of β-HCH areshown in Fig. 1.
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Table 1 Mean consumptions (g) of food groups among socio-economic sections
Foods HIGa mean (SD) MIGb mean (SD) LIGc mean (SD) Ind. laborers mean (SD) Slum dwellers mean (SD)
aHigh income groupbMiddle income groupc Low income group
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Discussion
Concentrations of pesticides
The lipophillic nature of the organochlorine chemicalsenables them to persist in environment for longer time,even after their discontinued use. They gradually find
their way into the food chain leading to several adversehealth effects (Kalpana 1999). In India, there is dearthof regular surveillance of the dietary intake estimates ofthese residues.
The levels of residues like DDT, HCH and aldrin infoods were lesser in the present study as also reportedby Bhushan (2006). DDT, HCH, cypemethrin,
Table 3 Median, 25th, and 75th percentile concentrations (μg/kg or μg/L) of pesticide residues in foods collected from 13 markets inHyderabad
Foods (N=13foreach food item)
Residuesdetected
No. of samplesdetected with residuesabove detection limit
Median concentration(mg/kg or L)
Range from 25th to 75thpercentile concentrations
MRLs by FSSAI(mg/kg or L)
Rice γ-HCH 3 0.0001 0.0001–0.0001 0.05
o′p′-DDD 4 0.0001 0.0001–0.0001 –
o′p′-DDE 4 0.0001 0.0001–0.0001 –
Wheat Flour γ-HCH 4 0.0044 0.0001–0.0935 Should be absent
o′p′-DDE 4 0.0001 0.0001–0.0001 –
Red gramdhal α-Endosulfan 3 0.0001 0.0001–0.0185 0.20
Green chilli α-Endosulfan 5 0.0001 0.0001–0.0001 0.20
Cypermethrin 13 0.293 0.13–0.39 3.5
MRLs maximum residue limits
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endosulfan, and aldrin (including dieldrin) in cookedvegetables were lesser than the concentrations shownin earlier samples collected from and aroundHyderabad (Reddy et al. 1998) and in Delhi (Bakoreet al. 2002). Presence and concentrations of HCHisomers and DDT metabolites were shown to decreasein many foods by Pandit et al. (2002) as compared toearlier study by Kalra et al. (1999). They were stilllesser in the present study. Milk samples in our studywere detected with higher concentrations of only β-HCH; whereas, in earlier studies (Battu et al. 1989;Kalra et al. 1999; Pandit et al. 2002), other isomers ofHCH (α, γ, δ) were also simultaneously found. Similarwas the case with DDT metabolites where traces ofonly o′p′DDTwere found in milk samples in our study
while all other metabolites were also detected in earlierstudies (Battu et al. 1989; Kalra et al. 1999; Pandit et al.2002). The trace presence of β-HCH instead of lindanein fish samples as shown in earlier studies (Kannanet al. 1992) may be due to its more persistent naturethan lindane and suggests its gradual phase offphenomenon.
All the water samples were detected with only β-HCH, but at levels (54.37 to 431.03 μg/L) were muchhigher than the permissible limits by the Bureau ofIndian Standards (BIS 2004) of 1 μg/L and the desir-able limit for pesticides in drinking water is given as“absent.” The levels also exceeded the limits for EU,much lower as the maximum admissible concentrationat 0.1 μg/L for individual pesticide and 0.5 μg/L for
Table 4 Estimated daily intakes of pesticide residues and their percent ADIs at mean levels of food intake among five socio economicsections in Hyderabad
a High income groupbMiddle income groupc Low income groupd Industrial laborerse Slum dwellersfμg/kg bw/d, microgram per kilogram body weight per dayg Acceptable daily intakes
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total allowable pesticide residue. Higher levels of β-HCH in milk and drinking water samples need furtherinvestigation.
All vegetables, except spinach, contained lesserconcentrations of OCPs when compared with earlierreported studies, probably due to the imposed ban ondirect spraying on fruits and vegetables. Leafy vegeta-bles also were reported to be affected with OCP resi-dues (Sasi and Sanghi, 2001); but in the present study,though the vegetables were detected with many resi-dues, they were all in trace quantities, not contributingsignificantly to the exposures.
The concentrations of HCH and DDT isomers inwheat flour samples were many folds below their re-spective MRLs. There are no statutory limits forDDT in cereals grains in India. However, the ricesamples were detected with trace presence of o′p′DDE, o′p′ DDD, and p′p′ DDT. Trace residues oflindane and o′p′ DDE were also detected in wheat
Table 5 Estimated daily intakes of pesticide residues and their percent ADIs at 95th percentile levels of food intake among fivesocioeconomic sections in Hyderabad
a High income groupbMiddle income groupc Low income groupd Industrial laborerse Slum dwellersfμg/kg bw/d, microgram per kilogram body weight per dayg Acceptable daily intakes
11.3
16.4
16.1
16.4
10.9
10.572.6
75.9
77.6
78.9
83.6
0% 20% 40% 60% 80% 100%
HIG
MIG
LIG
IL
SD
rice
wht flr
pulse
tomato
lf
potato
spinach
amaranth
mango
milk
water
fish
gr chillie
Fig. 1 Percent contribution to EDIs of β-HCH by various foodsin various SES
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flour samples exceeding the MRL of zero inmilled cereal grains.
Dietary intakes
The dietary intakes of organochlorines like DDT,HCH, aldrin, and diedrin through various foods inIndia were higher than those in many developed coun-tries (Kannan et al. 1992; Kashyap et al. 1994). Thecontribution of dairy products to the dietary intake ofthese residues was very high. In the present study, ahigher contribution was that of drinking water.Exposures to organochlorine pesticides (HCH andDDTs) through rice and wheat have been shown to beof very less magnitude by Toteja et al. (2003, 2006).
However, the estimates were higher for β-HCHresidue, in the present study, where the foods weremade as table ready. Higher estimates of intakes forβ-HCH were obtained not only due to the residuecontent of the raw foods but also of water, which isadded to the foods while cooking. Drinking waterimparted its residues to the cooked foods and elevatedtheir concentrations even though the raw foods werefree from the residues. The drinking water is suppliedto the entire city either from river Krishna and orManjira through municipal supply but the cause ofresidue levels in drinking water samples needs furtherinvestigation. Contamination of ground water inHyderabad with various concentrations of DDT, beta-Endosulfan, alpha-Endosulfan, and lindane, leading toexposures exceeding the ADIs, has been reported ear-lier (Shukla et al. 2006).
The amount of water added depended on the amountof food consumed. Population of lower socioeconomicsections in Hyderabad consumed significantly morecooked rice, and hence, more water was used forcooking. Therefore, EDIs of β-HCH by the populationof lower SES were much higher than MIG and HIG.
In an earlier study, in Kanpur, India (Shukla et al.2002), the daily intake of aldrin in average vegetariandiet exceeded ADI by 442 % and in average non-vegetarian diet by 1,500 %. The daily dieldrin intakein average vegetarian diet exceeded ADI by 514 % andin average non-vegetarian diet by as much as 6,000 %.The percent contributions in our study were muchlower than the above-mentioned study. In another stud-y (AICRP 2001), 75 % of the vegetarian diets wasfound to contain various concentrations of differentpesticide residues, and DDT and HCH residues were
detected in foods from all over the country. About 11 %of diets contained residues exceeding the ADIs. Non-vegetarian samples (72 %) were detected with HCH,DDT, endosulfan and chlorpyrifos, and 15 % wasexceeding the ADIs.
When comparing the trend of two residues commonfor analyses in our study with those reported from thefirst Hong Kong first TDS (HKTDS, 2012), the organ-ophosphate residue, chlorpyphos, and the syntheticpyrethroid, cypermethrin, were mostly found in vege-tables. Cypermethrin in Cameroon TDS (Gimmouet al. 2008) and chloropyriphos in French TDS(Nougadère et al. 2012) were also frequently presentin vegetables. These results were similar to our find-ings indicating similarity in their usage among thesouthern Asian countries. EDIs for chloropyriphos inthe present study were lower than the ADIs, but thepercent contribution to ADIs was greater than thoseobserved in the HKTDS (0.01–0.041 % of ADI). Thepercent contributions to ADIs for cypermethrin alsowere higher (0.4–8.71 % of ADI) in our study ascompared to the HKTDS (0.3–1 % of ADI). Unlikein the French TDS, where dieldrin and heptachlor werefound to be probable reasons for chronic risk at upperbound levels of residue concentrations in foods, theseresidues were not detected above the limits in our studyand their EDIs (when calculated with LOD as thenumeric for concentration) also were well below theADIs. Another study indicated reduction in ΣDDT inthe total diet but EDI levels exceeding the ADIs forlindane, mainly due to consumption of milk (Battuet al. 2005).
However, in the present study, cooking oil was notanalyzed which could have affected the EDIs as earlierstudies (Kannan et al. 1992) have shown high concen-trations of HCH and DDT isomers in groundnut oilsand ghee. The amount of cooking oils consumed alsowas found to be higher than many other foods.
Conclusions
Most of the residues were present at below detectablelevels in the most commonly consumed foods in vari-ous SES and those present above detection levels werein trace quantities with an exception of levels of β-HCH in water and milk. Absence of aldrin, dieldrin,heptachlor, chlordane, and α-HCH from the food sam-ples suggests clearance of these residues from local
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food chain, though it was evident that the use of otherresidues like α-endosulfan, chlorpyriphos andcypermethrin is on rise. EDIs below the respectiveADIs of residues suggest low chronic dietary expo-sures of the population of Hyderabad. However, levelsof β-HCH in water and milk samples prompt the needfor further investigation.
Acknowledgments This work was supported by a grant pro-vided by the Indian Council of Medical Research (grant number09-FD06) and University Grants Commission, Govt. of Indiaprovided the fellowship (Senior Research Fellowship) to AB.
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