The Swedish Monitoring of Pesticide Residues in Food of Plant Origin: 2005

Transcription

1 Rapport The Swedish Monitoring of Pesticide Residues in Food of Plant Origin: 2005 EC and National Report by Arne Andersson, Anders Jansson and Anna Hellström Bild: Ina Agency Press AB, Stockholm LIVSMEDELS VERKET NATIONAL FOOD ADMINISTRATION, Sweden

2 The Swedish Monitoring of Pesticide Residues in Food of Plant Origin: 2005 Report concerning Directives 90/642/EEC, 86/362/EEC and Commission Recommendation 2005/178/EC By Arne Andersson, Anders Jansson and Anna Hellström Further information Information about the Swedish monitoring of pesticide in food of plant origin is available from: Arne Andersson National Food Administration Box 622, SE Uppsala, Sweden Fax:

3 2 Livsmedelsverkets rapport nr 13/2006 National Food Administration, Sweden

4 CONTENTS Summary 5 Introduction 6 Monitoring programme 7 Sampling procedures 8 Analytical methods 9 levels 11 Maximum Residue Limits 11 Results and discussion 12 Dietary Exposure Assessment 20 References 32 Appendix 1 Analytical method codes and their sources 34 Appendix 2 Pesticides, isomers and breakdown products sought and detected 37 Appendix 3 surveillance grouped by analytical methods used 41 Appendix 4 Appendix 5 surveillance analysed and found in per cent of s enforcement analysed and found in per cent of s Tables according to EU reporting format: Table A1- Part I Table A1-Part II Table A1-Organic Table A2-Part I Table A2-Part II Table B Summary of numbers of analysed, sample origins and results, surveillance sampling, national and co-ordinated programme Summary of numbers of analysed, sample origins and results, enforcement sampling, national and co-ordinated programme Summary of numbers of analysed and results, surveillance and enforcement sampling, national and co-ordinated programme Fruit & vegetables: Summary table of pesticides sought and found, surveillance sampling, national and co-ordinated programme Cereals: Summary table of pesticides sought and found, surveillance sampling, national and co-ordinated programme Notifications of the co-ordinated programme (specific exercise) to the European Commission National Food Administration, Sweden Livsmedelsverkets rapport nr 13/2006 3

5 CONTENTS Table C Table D1 Table D2 Table D3 Table D4 Table E Continue Notifications of the results of Check sampling (Surveillance sampling) of the National programme to the European Commission. The results include the in the co-ordinated programme Details of exceeding EC-s, surveillance sampling of fruits, vegetables and cereals, national and co-ordinated programme Details of exceeding non-harmonised s including national s, surveillance sampling of fruits, vegetables and cereals, national and co-ordinated programme Details of exceeding EC-s, follow-up enforcement sampling of fruits, vegetables and cereals, national and co-ordinated programme Details of exceeding non-harmonised s, including national s, follow-up enforcement sampling of fruits, vegetables and cereals, national and co-ordinated programme Details of with multiple (>2) in single, surveillance and follow-up enforcement sampling of fruits, vegetables and cereals, national and co-ordinated programme Table F Details of the homogeneity exercise 219 Table G Laboratories: Information about laboratories involved in the monitoring exercise Livsmedelsverkets rapport nr 13/2006 National Food Administration, Sweden

6 The Swedish Monitoring of Pesticide Residues in Food of Plant Origin: 2005 EC and National Report Summary In 2005, a total of surveillance of fresh, frozen or processed fruits and vegetables, cereal grains and cereal products were analysed for of 253 pesticides (302 analytes). National or EU harmonised Maximum Residue Limits were exceeded by 89 (4.2 %). Reidues above the s were found in 5.6 % out of of fresh or frozen fruits and vegetables. The violation rate shows a slight increase compared with 2004 and amounted to 8.1 % in fresh or frozen fruits and vegetables from third countries and 5.1 % in the from EU countries except Sweden. Only one of the of domestic grown fruits and vegetables contained above the s. No were found in any of the 20 from organic production. The frequency of containing was roughly the same in domestic Integrated Production (IP) compared with domestic convential production. Pears, beans, potatoes, carrots, oranges, mandarins, spinach, rice and cucumber, in all 529, were analysed in the 2005 EU co-ordinated programme. Twenty of these exceeded any of the EC-s for the 56 pesticides concerned. In ten commodities (12 ) pesticide were found at levels more than 10 times the s. The highest violation rate, 81 times the, was found in litchis from Israel containing prochloraz. No were found in the 95 of foods for infants and young children. A total of 247 of cereal grains were analysed. Most of the (81 %) contained no and none of exceeded any s. In the enforcement sampling of fruits and vegetables 68 were collected and 13 lots (28.2 tons) were prohibited from being sold. The homogeneity factor, calculated as the highest value found in an individual unit divided by the mean residue of individual units in a single sample, was determined for dimethoate and omethoate in lettuce. The short-term intake was estimated for the acute toxic pesticides based on the highest residue found in a surveillance (composite) sample. The ARfDs were exceeded for toddlers in six cases. The chronic (long-term) intake was estimated using monitoring data from Of the 22 pesticides included in the calculations dicofol reached the highest intake, 12 % of the ADI when the most conservative estimate was applied. National Food Administration, Sweden Livsmedelsverkets rapport nr 13/2006 5

7 Introduction The Swedish National Food Administration (NFA) checks foods of plant origin for pesticide. Annual reports have been published in English since The present report is our seventh combined European Commission (EC) and national report. It is aimed for the Commission, the Member States in the European Union (EU) and all other interested parties. The report contains general information about the monitoring programme, sampling procedures and analytical methods as well as detailed information about found using a format requested by the European Commission (Table A G). Certain results are also presented in percent of the s according to our general format for reporting found (Appendices 4 5). Responsible for the method development has been Tuija Pihlström at the National Food Administration. The validation of the analytical methods has been done under supervision of Paula Friman at the contracted laboratory, Lantmännen Analycen AB in Lidköping. All have been analysed at this laboratory under management of Annelie Lundh. An assessment of the short-term intake, based on the 2005 monitoring data, has also been carried out. Further more, this report contains also a calculation of the chronic intake for 22 pesticides based on monitoring data from Bengt-Göran Ericsson and Petra Fohgelberg at the National Food Administration have done the calculations and presentation of these results. This report is available on NFA s web site together with a separate comprehensive summary report in Swedish. Since 2001 quarterly and from 2004 tertiary summary reports from the pesticide monitoring are also available in Swedish on NFA s web site: 6 Livsmedelsverkets rapport nr 13/2006 National Food Administration, Sweden

8 Monitoring programme The target number of to be collected of each food takes into account the food's consumption rate. However, less are taken of commodities causing only few exceedances of the s. The number is also based on the importance of the foodstuff in the diets of infants and young children and if the food is consumed with or the peel. In some cases, the number of of a specific food or a food from a particular country was increased based on found in prior. By analysis of 100 it can with 95 % confidence be predicted that the actual percentage of exceedances is less than 3 % provided that no exceedances was discerned. About 100 different commodities were included in the sampling plan for year 2005 (Table 1 and Table C). Table 1. and commodities to be collected according to the monitoring programme 2005 and the outcome of the sampling. COMMODITY No. of 2005 COMMODITY No. of 2005 planned outcome planned outcome Fruits (fresh or frozen) Onions Apples Peppers Bananas Potatoes Mandarins and similar Others Oranges Peaches and nectarines Cereal grains Pears Rice Strawberries Wheat Table grapes Others Others Processed or dried foods Vegetables (fresh or frozen) Baby foods Carrots Cereal products Cucumbers Juice, fruit drinks Head cabbage Potatoe products Lettuce Others Melons Tomatoes Total: National Food Administration, Sweden Livsmedelsverkets rapport nr 13/2006 7

9 Sampling procedures Surveillance monitoring Samples collected in accordance with the monitoring programme are defined as surveillance, i.e. there are no suspicions about excessive amounts of pesticide in the lots prior to sampling. Enforcement sampling When a surveillance sample contained a pesticide residue above the national or EC maximum residue limit (1-2), the NFA prescribed a condition for the offering for sale or other handling of the food or lot to which the food belonged. As a follow-up, next lots of the commodity from the grower/ exporter were detained and enforcement were collected. The condition was cancelled either when a certain number of lots contained pesticide below the s, or when other information showed that the residue problem did not exist any longer. Surveillance sampling was then once more resumed. Sample collection Fresh fruit and vegetables were sampled at wholesalers' warehouses in the first trade channel. The sampling was done according to the EC sampling method described in Commission Directive 2002/63/EC (3). The sample was sealed and labelled with a unique sample identity. Most of the of processed or frozen fruit and vegetables, juices, fruit drinks, rice, cereal products and vegetable oils were collected in retail shops or department stores. Samples of domestic produced cereal grains were collected at the milling plants. The imported cereal grains were sampled at the port where the shipment was discharged. Usually, one bulk sample of about 3 5 kg was collected by stream sampling technique. Plant inspectors from the National Board of Agriculture collected most of the, but inspectors from the Municipal Environmental and Health Protection Committees were to some extent also involved. Quality assurance measures Trained inspectors belonging to the National Board of Agriculture collected the according to written instructions from the National Food Administration. The bags with the were sealed and a photo was taken of the box that had been sampled. 8 Livsmedelsverkets rapport nr 13/2006 National Food Administration, Sweden

10 Analytical methods Method development and validation Tuija Pihlström, National Food Administration Paula Friman, Lantmännen Analycen AB Most of the method development is done by the National Food Administration (NFA). Validation of the methods is carried out by both NFA and Lantmännen Analycen AB (ALC). The close co-operation between NFA and the highly competent laboratory staff at the contracted laboratory ALC allows a quick and trustworthy transfer of the methods for monitoring of pesticide. The multi-residue method has been revised and improved continuously and its scope has been extended (Table 2 and Figure 1). During the recent years efforts have been made to simplify the multi residue method. The result is an improved methodology for analysis of pesticides in matrices with different ph by adding NaHCO 3 prior to the extraction step. Furthermore, the introduction of LC-MS/MS technique has made it possible to replace many single methods, providing higher sensitivity and proof of identity. Table 2. Pesticides added to the multi method (M200) for fruit and vegetables in The reporting limit (RL) is 0.01 mg/kg for all the pesticides except abamectin for which the RL is 0.05 mg/kg. Dimethomorph Abamectin Fenpiclonil Methabenzthiazuro n Fenhexamide Chlorbromuron Flucytrinat Propamocarb Spiroxamin Difenconazole Iprovalicarb Tebuconazole Tetraconazole Famoxadon Isoproturon Tebufenozid Pesticide coverage In all, by using both multi residue methods (MRM) and single residue methods, it was possible to determine 253 pesticides corresponding to 302 analytes including metabolites and degradation products (Appendices 2 3). This is an increase with 14 pesticide compared with 2004 (4). By using LC-MS/MS it has been possible to lower the limit of quantification (LOQ) to 0.01 mg/kg for a large number of pesticides. The analytical method codes and their sources are listed in Appendix 1. A total of about (analyte/commodity combinations) were sought (Table A2-Part I and II). Fruit and vegetables The analysis of pesticide in fruit and vegetables is carried out using the multi residue method (M200) based on the extraction with ethyl acetate and determination with conventional GC detectors and LC-MS/MS. A total of 226 pesticides and 274 compounds were covered by this method. The addition of NaHCO 3 as alkaline to all commodities/analytes combinations allows the extraction of all included analytes in different matrices in one extraction. National Food Administration, Sweden Livsmedelsverkets rapport nr 13/2006 9

11 The development of using GC-MS/MS in the multi residue method is in progress and will further simplify the method by replacing the conventional GC detectors and reduce or get rid of the need of clean up. In addition to four MRMs also eleven single residue methods were used, and in all 249 pesticides (297 analytes) were sought in fruits and vegetables. Of these pesticides, 112 were actually found. Figure 1 shows number of analysed and pesticides sought and detected during the last six years No. of No. of pesticides No. of pesticides sought No. of pesticides detected No. of Figure 1. pesticides (active substances) sought and detected, and number of of fruit and vegetables analysed, surveillance sampling Vegetable oils The were extracted using hexane and acetonitrile. After clean-up on an S-X3 gel permeation column the were determined by GC equipped with ECD, FPD or N/P-detector. A total of 32 pesticides (37 analytes) were covered by the method used (code 018). Cereal grains and cereal products All of cereal grains and cereal products were analysed using MRM code 901. Single residue methods were used for analyses of chlorme-quat, mepiquat, inorganic bromide, hydrogen phosphide, glyfosate and AMPA. In all, 43 pesticides (52 analytes) were included in the control of cereals. 10 Livsmedelsverkets rapport nr 13/2006 National Food Administration, Sweden

12 Quality control Among other procedures, the quality control included daily checks of the instruments' sensitivity by injection of test solutions. GC-determinations were in most cases carried out using standards in matrix extracts. The EC guidelines Quality Control Procedures for Pesticide Residue Analysis (5) have been implemented as far as possible (Table G). The laboratory has participated in one proficiency test organised by EU and in 23 tests organised by FAPAS (UK), NFA (Sweden), DFVF (Denmark) and MUVA (Germany), see Table G. Laboratory used and accreditation The analyses were carried out on a contract basis at AnalyCen Nordic AB, Lidköping. In April 2006 the laboratory changed name to Lantmännen Analycen AB. This laboratory is accredited by the Swedish accreditation authority SWEDAC for all analytical methods used for the NFA s official control of pesticide in food of plant origin. levels The majority of the pesticide were measured and reported from the limit of quantitation (determination), generally in the range of mg/kg. levels for each of the pesticides are given in Table A2-Part I-II. For certain pesticides the EC-s set at the LODs (Limit of Determination) were not achievable in our routine monitoring. Maximum Residue Limits The National Food Administration's Regulations on Pesticide Residues in Food, sets s for about 280 individual substances or group of substances (according to the residue definition in the regulation). Fresh, frozen and dried fruits and vegetables, cereal grains, some cereal products as well as baby foods are covered by the regulations (1-2). The s, national and EC-s, apply equally to domestic, EU and third country commodities, whether or not the pesticide is authorised in Sweden. When regulations concerning a certain pesticide or a certain group of food products are not given in the regulations, the NFA can decide the maximum level to be applied in each individual case. National Food Administration, Sweden Livsmedelsverkets rapport nr 13/

13 Results and discussion Surveillance monitoring In 2005, a total of surveillance of fresh, frozen or processed fruit and vegetables, cereal grains and cereal products were analysed for pesticide. National and EU harmonised Maximum Residue Limits (EC-s) were exceeded by 89 (4.2 %) of these (Table A1-Part I and Tables D1-2). Table 3 shows the number of surveillance analysed by country of origin. About 70 % of the originated from foods from 59 foreign countries. Most of the with unknown origin came from processed products. In 2004, the number of amounted to originating from 61 countries (4). Out of of fresh or frozen fruits and vegetables 896 (57 %) contained at or below national and EC-s and 89 (5.6 %) exceeded these limits. None of the 247 of cereal grains exceeded the s and 81 % contained no at all. In all, analyses were carried out using 15 analytical methods. The number of surveillance analysed by the different analytical methods and arranged by food-groups is shown in Appendix 3. Out of the 253 pesticides (active substances) sought in all foodstuffs 115 were actually detected. The total numbers of findings of each pesticide in fruits, vegetables and cereal grains are shown in Table A2-Part I-II. Table 3. Total number of surveillance by country analysed in Country No. of Country No. of Country No. of Argentina 78 Guatemala 2 Norway 3 Australia 5 Honduras 2 Pakistan 7 Austria 2 Hungary 7 Panama 9 Belgium 20 India 15 Peru 13 Brazil 89 Israel 64 Poland 20 Canada 2 Italy 154 Republic of Korea 1 Chile 35 Jordan 1 Senegal 2 China 31 Kazakhstan 2 South Africa 77 Colombia 50 Kenya 8 Spain 166 Costa Rica 31 Latvia 2 Swaziland 1 Croatia 1 Lebanon 3 Sweden 561 Cyprus 17 Madagascar 1 Syrian Arab Republic 1 Czech Republic 1 Makedonia 1 Thailand 54 Denmark 10 Malaysia 1 Turkey 62 Dominica Rep. 2 Mali 1 United Kingdom 17 Ecuador 12 Mauritius 1 United States 87 Egypt 21 Mexico 2 Unknown country 101 France 21 Morocco 35 Uruguay 12 German 29 Namibia 3 Zimbabwe 5 Fed.Rep. Ghana 1 Netherlands 90 Greece 14 New Zealand 30 In total Table D1 gives detailed information about pesticide found and action taken for those 82 surveillance of fruits and vegetables that exceeded EU harmonised s. In 15 of the, two or more pesticides exceeded the EC- s in the same sample. Two of those contained even three pesticides above the limits. 12 Livsmedelsverkets rapport nr 13/2006 National Food Administration, Sweden

14 Information about pesticide found and action taken for those seven surveillance of fruits and vegetables that exceeded non-harmonised s is given in Table D2. Out of of fruit, vegetables and cereal grains (surveillance and compliance) 587 (31 %) contained of two or more pesticides in a single sample. The highest number of pesticides found was nine and these were found in one sample of pears from Italy and two of table grapes from Italy. Eight pesticides were found in one sample of table grapes from Italy. Detailed information is given in Table E for all with two or more pesticide in a single sample. The most commonly found pesticides in fresh or frozen fruit, vegetables and cereal grains are presented in Table 4. The fungicides imazalil and thiabendazole were among those most often found in fruits, while imidacloprid and carbendazim were most often found in the vegetable. Out of the eight different pesticides detected in cereal grain, the growth regulators chlormequat and mepiquat were most often found. Table 4. Pesticides most commonly found in fresh or frozen fruits and vegetables and cereal grains, surveillance sampling in Fruits Vegetables Cereal grains (922 ) (660 ) (247 ) No. of No. of No. of Pesticide findings Pesticide findings Pesticide findings Imazalil 252 Imidacloprid 53 Chlormequat 21 Thiabendazole 245 Carbendazim 29 Mepiquat 13 Carbendazim 165 Dithiocarbamates 23 Phosphine 11 Carbaryl 71 azoxystrobin 22 Glyphosate 7 Chlorpyrifos 60 Procymidone 21 Bromide (inorganic) 3 Dithiocarbamates 52 Propamocarb 21 Pirimiphos-methyl 2 Iprodion 52 Chlorothalonil 19 Deltamethrin 1 Orthophenylphenol 52 Imidacloprid 19 Malathion 1 Captan 50 Endosulfan 17 Chlorpyriphos 43 Cypermethrin 16 Comparison of from different types of production system The total number of analysed from organic, integrated (IP) and conventional production was 20, 196 and 1 880, respectively (Table 5). None of the from organic growing contained. 55 (28 %) from domestic Integrated Production (IP) contained but none exceeded the s. Out of the 361 from domestic conventional production 76 (21 %) contained. One of these exceeded the s. In general, the frequency of containing pesticide was more or less the same in domestic Integrated production compared with domestic conventional production. National Food Administration, Sweden Livsmedelsverkets rapport nr 13/

15 Table 5. Comparison of found grouped by type of farming, surveillance sampling in Type of production Origin Total no. of No of containing No Residues< Residues > Organic Domestic Import IP Domestic Import Conventional Domestic Import Fruits and vegetables - fresh or frozen A total of of fresh or frozen fruit and vegetables including potatoes were analysed for of 249 pesticides (297 analytes including metabolites and degradation products). About 38 % of the contained no. National or EC-s were exceeded in 89 (5.6 %) of the (Figure 2). The number of exceedances in 2004 was 77 (4.4 %). Fruit & Vegetables Total % 32.5% Sweden % EU except Sweden % 35.2% Third countries % 27.3% 37.7% 67.2% 59.8% 64.5% 56.6% Residues above national or EC-:s Residues at or below national or EC-:s Without Figure 2. Summary of results for fresh or frozen fruit and vegetables, surveillance sampling in In general, the imported commodities contained considerably more often than the domestic. Most (67 %) of domestic grown fruit and vegetables contained no. The corresponding figures for EU-countries (except Sweden) and third countries were 35 % and 27 %, respectively. Only one (0.3 %) of the of domestic grown fruits and vegetables exceeded national or EC-s compared with 5.1 % of the from EU countries (except Sweden) and 8.17 % from third countries. surveillance of each fruit and vegetable and the pesticide found (in per cent of the ) are presented in Appendix Livsmedelsverkets rapport nr 13/2006 National Food Administration, Sweden

16 Commodities containing pesticide greater than 10 times the are shown in Table 6. The ratio between the highest level found in the surveillance sample and the is given. Residues of prochloraz in a sample of litchis from Israel amounted to 81 times the. However, the high figures are partly due to cases where the s are set at the limit of determination. Table 6. Commodities containing pesticide greater than 10 times the, surveillance sampling in Commodity Pesticide Country No. of Max. Ratio of origin with residue mg/kg max. >10 found residue/ times mg/kg Litchis Prochloraz Israel Figs Dithiocarbamates Brazil Beans, with pods Dimethoate Thailand Coriander Profenfos Thailand Papayas Imazalil Brazil Chinese Broccoli Profenfos Thailand Chinese Broccoli Cypermethrin Thailand Mandarins Dimethoate Spain Melons Acephate Brazil Passion Fruits Dithiocarbamates Kenya Beans, with pods Dimethoate Egypt Chinese Broccoli Lambda-Cyhalotrin Thailand Papayas Chlorothalonil Brazil Oranges Dimethoate Egypt EU co-ordinated programme The EU co-ordinated programme for 2005 consisted of nine commodities and 56 pesticides (6). The minimum number of per commodity to be analysed by each of the member states was 12 to 93 depending on the population size in the MS. In Sweden the EU co-ordinated programme is included in the national monitoring programme. In all, 529 of pears, beans, potatoes, carrots, oranges, mandarins, spinach, rice and cucumber were analysed (Table B). Residues above the EC-s for the pesticides listed in Table B were found in seven out of the 36 of beans, three out of the 62 of cucumbers, two out of the 65 of mandarins, five out of the 70 of oranges and in three out of the 20 of spinach. None of the of carrots, pears, potatoes and rice contained above the EC-s (Figure 3). The EU co-ordinated programme included also analysis of individual units of pears, potatoes, carrots, oranges, mandarins, and cucumbers for pesticides posing an acute risk, e.g. OP-esters endosulfan and N-methylcarbamates. The homogeneity factor has to be calculated based on the in the individual units. No investigations were possible to carry out as none of the taken contained National Food Administration, Sweden Livsmedelsverkets rapport nr 13/

17 for those combinations. However, the homogeneity factor has been determined for dimethoate and omethoate in lettuce. The figures were 1.7 for dimetheoate and 1.2 for omethoate. The result is shown in Table F. A total of 95 of different baby foods such as beverages, fruit purées, vegetable purées, gruels and porridge have been analysed. None of the contained pesticide at or above the reporting level of 0.01 mg/kg (Table C). Finally, from produce originating from organic farming should also be taken within the EU co-ordinated programme. In all, 20 were analysed and none of them contained (Table A 1-Organic). Percentage of number of 100% 80% 60% 40% 20% 0% No Residues below s Residues above s Beans Carrots Cucumber Mandarines Oranges Pears Potatoes Rice Spinach Commodity Figure 3. Summary of results for the EU co-ordinated programme, only EC-s and pesticides included in Table B, surveillance sampling in Violation rates of pesticide The frequency of of fresh or frozen fruits and vegetables with pesticide above national or EC-s is shown in Figure 4. The violation rate has slightly increased and amounted to 8.1 % in fresh or frozen fruits and vegetables from third countries and 5.1 % in the from EU countries except Sweden. Only one of the of domestic grown fruits and vegetables contained above the s. 16 Livsmedelsverkets rapport nr 13/2006 National Food Administration, Sweden

18 Exceedances 12% 11% 10% 9% 8% 7% 6% 5% 4% 3% 2% 1% 0% Sweden EU (excl. Sweden) Third countries Figure 4. Violation rate of pesticide in of fresh or frozen fruits and vegetables, national or EC-s, surveillance sampling during Foods intended for infants and young children In total, 95 of baby foods e.g. cereal based product, juices, fruit drinks, canned fruits and vegetables were analysed. No detectable were found in any of the. Juices and fruit drinks (excluding baby food ) A total of 47 of juices and fruit drinks were analysed. Six of the contained. Three of the nine of grape juice contained 0.02 mg/kg of carbaryl and carbendazim. In one of nine of apple juice 0.02 mg/kg of carbendazim was found. Thiophane methyl, 0.05 mg/kg, was found in one of nine of tomato juice. Fruits and vegetables processed or dried (excluding baby food ) 66 of dried fruits and canned or processed vegetables were analysed. In three of the 34 of canned fruits and vegetables were found. Eleven out of the 15 of dried fruits contained pesticide. The sprout inhibitor chlorpropham was found in nine out of 18 of fried potato products. One sample of potato crisps contained 2.7 mg/kg of chlorpropham. Detailed information is given in Table C. National Food Administration, Sweden Livsmedelsverkets rapport nr 13/

19 Vegetable oils Olive oil, 14 in all, were analysed for of 32 pesticides (method code 018). Endosulfan was detected in seven of the and the highest residue found was 0.07 mg/kg (Table C). Cereal products A total of 38 of pasta, were analysed. None of the contained (Table C). Cereal grains A total of 247 of cereal grains, mainly wheat, rice and rye, were analysed. None of the exceeded the s and most of the (81 %) contained no at all (Figure 5). Nine out of 53 of rice contained hydrogen phosphide. The highest residue was mg/kg. The growth regulators chlormequat and mepiquat were most frequently found pesticides in cereal grains (Table 4). Chlormequat was found in 21 out of the 23 of rye, at 0.84 mg/kg as the highest residue (Table C). Cereal grains 19.0% Total % Sweden % 0.0% EU except Sweden % 0.0% Third countries % 28.8% 86.2% 72.7% 71.2% Residues above national or EC-:s 81.0% Residues at or below national or EC-:s Without Figure 5. Summary of results for cereal grains, national or EC-s, surveillance sampling in Enforcement Enforcement were collected as a follow-up, when excessive amounts of pesticide were found in surveillance. National and EC-s were exceeded in 27 out of 68 enforcement (Table A1-Part II and Tables D3-4). A total of 13 lots (28.2 tons) of foods were prohibited for sale in 2005 (Table 7), compared with 14 lots (35.8 tons) in 2004 (4). These lots had either to be destroyed or returned to the supplier. A re-export is accepted only when the competent authority in the receiving country gives its approval. The number of analysed, grouped by food commodity, country of origin and found, expressed in per cent of the, are shown in Appendix Livsmedelsverkets rapport nr 13/2006 National Food Administration, Sweden

20 Table 7. Lots prohibited for sale in 2005 Food Country No. of lots Weight, ton Chinese kale Germany Coriander Thailand Mandarins Spain Papaya Brazil Passion fruits Kenya Sharon fruits South Africa Spinach Spain Total Rapid Alert System The Rapid Alert System for Foodstuffs (RASFF) was established by Council Directive 92/59/ECC on General Product Safety. Products entailing a serious health risk to the consumer are classified as Alert notifications. The notifying Member State (MS) informs the Commission, which then notifies the other Member States. Sweden has during 2005 sent three food-alarms concerning high pesticide to the Commission. The notifications were: dithiocarbamates in Rucuola from Italy, prophenophos in Chinese Broccoli from Thailand and dimethoate/- omethoate in Cutting lettuce from Denmark. National Food Administration, Sweden Livsmedelsverkets rapport nr 13/

21 Dietary Exposure Assessment Homogeneity (variability) factor The homogeneity (variability) factor is defined as the quotient between the maximum and the mean residue of individual units in a sample. This factor was determined for dimethoate and omethoate in lettuce. In the calculations, units containing no were assigned a figure corresponding to half of the limit of determination. The homogeneity factor was 1.7 for dimethoate and 1.2 for ometoate in lettuce (Table 8 and Table F). Table 8. Homogeneity factors for pesticides/commodities investigated in Pesticide Commodity No. of units Homogeneity Max Mean residue, residue, factor mg/kg mg/kg Sample Reference Dimethoate Lettuce S311 Omethoate Short-term Intake The acute dietary intake or short-term exposure has to be considered for those pesticides that are classified as acute toxic. This area is relatively new and approaches how to estimate the acute intake has been put forward by WHO (7-10) and UK (11). The aim of the WHO and EU is to evaluate pesticides and establish acute reference doses (ARfD) for pesticides that possibly impose an acute health risk (12-13). The acute reference dose of a chemical is an estimate of the amount a consumer can ingest during one meal or during one day any health risk. In this study the national estimated short-term intake (NESTI) has been calculated for each pesticide found and for which EU, JMPR or JECFA have established a reference dose. The type of foodstuffs of most concern when estimating the acute exposure are those where the entire commodity (including peel) is consumed at one occasion, i.e. nectarines, apples or table grapes. Calculation of the national estimated short-term intake The national estimated short-term intake was calculated using the formulae shown in Figure 6. These formulae (case 2) are used when the meal-sized portion, as a single fruit or piece of vegetable (unit weight of the whole portion is > 25 g) might have a higher concentration of residue than the composite sample due to variability of in individual units. When the residue data reflect residue levels in the food as consumed (case 1), no variability factor is considered (i.e. cereals, juices). The consumption figures used when calculating the national estimated short-term intake (NESTI) are based on the 97.5 th percentile consumption of eaters only, which reflects the largest portion consumed during one meal or during one day. In this study consumption data from United Kingdom have been used (Table 9). Monitoring data reflect residue levels found in the products on the market. The observed residue (OR comp ) is the highest residue found in a composite sample. In order to refine the intake estimates, correction factors (when available) were applied 20 Livsmedelsverkets rapport nr 13/2006 National Food Administration, Sweden

22 to foodstuffs that normally are peeled or prepared, e.g. boiled or fried (11). OR comp is multiplied with a variability (homogeneity) factor (V). For commodities with unit weights between g a default factor of 7 (10 for leafy vegetables) is used. A factor of 5 is used for unit weights above 250 g. Known variability factors or in individual units should be used for more refined estimates. Table 9. Consumption figures and unit sizes for foods used in the short-term intake calculations (UK data). Commodity Large portion size Unit size Toddlers Adults (kg) (kg) (kg) Apples Beans (with pods) Cucumber Leek Lettuce Mandarins Mangoes Oranges Pears Peppers Pineapples Strawberries Table grapes Tomatoes National Food Administration, Sweden Livsmedelsverkets rapport nr 13/

23 Case 1: The composite residue data reflect residue levels in the food as consumed NESTI = LP ORcomp bw Case 2a: The unit weight of the whole commodity (U) is smaller than the large portion (LP) NESTI U = ORcomp V ( + LP U bw ) ORcomp Case 2b: The unit weight of the whole commodity (U) is larger than the large portion (LP) NESTI = LP ORcomp bw V NESTI = National estimated short-term intake U = Median unit weight of the edible portion (kg) OR comp V = = Highest observed residue in a composite sample of edible portion incorporation processing factors if available (mg/kg) Variability factor; 1 to 10 depending on unit weight and commodity LP = Highest large portion provided (97.5th percentile of eaters) in kg of food per day bw = Body weight (kg) Figure 6. The formulae used for calculating the national estimated short-term intake. 22 Livsmedelsverkets rapport nr 13/2006 National Food Administration, Sweden

24 Results of the assessment of the national estimated short-term intake Children, with low body weight relative to their consumption of fruits and vegetables, compose a risk group of approaching the acute reference dose (ARfD) when the products contain high levels of acute toxic pesticides. In this study the estimated short-term intake has been calculated for a large number of pesticides/commodity combinations. However, the results are shown only when the intake for a child/toddler is above 50 % of the ARfD (Table 10 and Figure 7). The estimated short-term intake for a child (body weight 14.5 kg) exceeded the ARfD for dimethoate/omethoate in lettuce, imazalil in oranges, chlorothalonil in tomatoes (two cases), oxamyl in cucumber and triazophos in pineapple (Figure 7). The intake of triazophos in pineapples from Costa Rica reached 9 times the ARfD for a child and three times the ARfD for an adult (Table 10). As no information was available for the distribution of triazophos between peel and pulp no correction factor could be applied. However, it is likely that this is an overestimate of the real intake. 200% 244% 877% 420% Per cent of ARfD 150% 100% 50% 0% Apples Beans (with pods) Cucumber Leek Lettuce Mandarins Mangoes Oranges Pears Peppers Pineapples Strawberries Table grapes Tomatoes Cyhexatin Dimethoate/Omethoate Imazalil Carbaryl Chlorothalonil Lambda-cyhalothrin Methiocarb Oxamyl Prochloraz Triazophos Figure 7. Estimated short-term intake for a child, surveillance sampling in National Food Administration, Sweden Livsmedelsverkets rapport nr 13/

25 Table 10. The estimated short-term intake of certain pesticides based on the highest residue found in composite in Only intakes above 50 % of the ARfD for a toddler are shown. Pesticide Commodity ArfD, mg/kg bw Highest residue, mg/kg Correction factor Homogeneity factor Intake, % of ARfD toddlers Adults Cyhexatin Pears Dimethoate/Omethoate Apples Apples Beans (with pods) Lettuce Lettuce Imazalil Oranges Oranges Oranges Oranges Oranges Oranges Oranges Oranges Oranges Oranges Oranges Apples Mandarins Mandarins Mandarins Mandarins Mandarins Mandarins Pears Pears Carbaryl Apples Apples Apples Chlorothalonil Apples Strawberries Leek Tomatoes Tomatoes Lambda-cyhalotrin Table grapes Methiocarb Peppers Oxamyl Cucumber Prochloraz Mangoes Triazophos Pineapples * *No correction factor found for triazophos 24 Livsmedelsverkets rapport nr 13/2006 National Food Administration, Sweden

26 Chronic intake Bengt-Göran Ericsson and Petra Fohgelberg, National Food Administration. The national estimated daily intake (NEDI) of pesticide from foods of plant origin was estimated using Swedish monitoring data from A total of 37 commodities and 22 pesticides, the same as in previous report (14), were included in the calculations. The results of the assessment was presented at the poster session of European Pesticide Residue Workshop (EPRW) 2006 (15). Commodities and consumption data The commodities included fruits, vegetables, cereals, vegetable oils and juices (Table 11). The chosen products from these groups are in most cases consumed in considerable amounts in Sweden, and are by experience known to contain pesticide. They are also represented in the previous estimations that have been reported in the year 1998, 1999, 2000 and 2001 (14, 16-18). The consumption figures were composed by domestic and imported foodstuffs. Consumption data for the domestic commodities were derived from several sources in the same manner as previous years, including for example the two Swedish dietary surveys carried out in 1989 and For imported foods the figures were based on import statistics derived from Statistics Sweden. The intake was calculated at the average and at the 90 th percentile consumption in order to include consumers with a higher consumption. Table 11 shows the consumption figures on a whole commodity basis. Furthermore, the percentage edible portion is given. Table 11. Average and 90 th percentile food consumption figures for the 37 foodstuffs included in the study of national estimated daily intake. Product Consumption (grams/day and person) 1 Edible Average 90th percentile portion Domestic Import Total Domestic Import Total % Fruits Apple Banana Grapefruit Grapes Lemon/lime Mandarin Orange Peach/ nectarin Pear Pineapple Strawberries Vegetables Aubergine Beans Cabbages Carrot Cauliflower Cucumber Leek Lettuce Melon, others National Food Administration, Sweden Livsmedelsverkets rapport nr 13/

27 Product Consumption (grams/day and person) 1 Edible Average 90th percentile portion Domestic Import Total Domestic Import Total % Onions Peas Pepper Potato Potato products Tomato Watermelon Cereals Oat Rice Rye Wheat Vegetable oils Olive oil Rapeseed oil Fruit juices Apple juice Orange juice The figures refer to whole commodity Calculation of the National Estimated Daily Intake (NEDI) The intake calculations were carried out on the basis of edible portion consumed and correction factors (when available) for the distribution of between e.g. peel and pulp (Table 12). The residue levels used in the calculations were determined according to a-c: a) average residue level, negative were assigned a zero value b) average residue level, negative were assigned the reporting level (RL) c) 95 th percentile residue level, negative were assigned the reporting level A certain pesticide/commodity combination was included in the intake estimation only if at or above the reporting level (Table 13) were found in at least one of the from that commodity. Otherwise the intake contribution from that pesticide/commodity combination was assumed to be zero. The national estimated daily intake (NEDI) was calculated using the following formula: NEDI = F i x R i x C i x P i F i = Food consumption of the relevant commodity (kg/day), subdivided in domestic and imported products R i = Pesticide residue level (mg/kg) in the foodstuff, derived from monitoring data (subdivided in domestic and imported products) C i = Correction factor for transforming on whole commodity to edible portion (e.g. bananas, citrus) P i = Correction factor that takes into account reduction or increase of the residue after commercial processing, preparation or cooking of the food 26 Livsmedelsverkets rapport nr 13/2006 National Food Administration, Sweden

28 Table 12. Correction factors used for refinement of the estimated intake. Pesticide Foodstuff Correction factor 1 All pesticides Peaches, nectarines 1.19 Benomyl group Citrus 0.43 Chlorpropham Potatoes/Chips (French fries) 0.80 Dicofol Citrus 0.03 Dimethoate/omethoat Mandarins 0.26 e - " - Oranges 0.26 Ethion Citrus 0.02 Imazalil Bananas " - Citrus " - Melons 0.10 Mecarbam Citrus 0.05 Methidathion Citrus 0.03 Thiabendazole Bananas " - Mandarins " - Oranges, lemons, limes, grapefruit Fraction of the residue in the edible part (16,19-21). Pesticides and ADI-values The acceptable daily intake (ADI) is the daily intake that, during a lifetime, appears to be appreciable risk, on the basis of all the facts known at that time. It is expressed in milligrams of the chemical per kilogram of body weight. A safety factor, usually 100, is included in ADI. The pesticides were selected from a risk perspective, i.e. low ADI-values and widely used on a variety of commodities. The established ADIs for the pesticides in this study are shown in Table 13. The ADI-values used are primarily from EU (after inclusion in Annex 1 of Directive 91/414/EEC), otherwise from JMPR (Joint FAO/WHO Meeting on Pesticide Residues). Table 13. levels and ADIs for the pesticides included in the national estimated daily intake. Pesticide level (mg/kg) ADI and source (mg/kg bw) Acephate 0.01/ (JMPR 2005) Azinphos-methyl (JMPR 1991) Benomyl group (Carbendazim) 0.01/ (JMPR 1995) Carbaryl 0.01/0.03/ (JMPR 2001) Chlormequat 0.01/ (JMPR 1997) Chlorpropham 0.05/ (EU 2003) Dicofol 0.05/ (JMPR 1992) Dimethoate/omethoate / (JMPR 1996) Diquat (EU 2001) Endosulfan 0.01/ (JMPR 1998) Ethion 0.01/ (JMPR 1990) National Food Administration, Sweden Livsmedelsverkets rapport nr 13/

29 Pesticide level (mg/kg) ADI and source (mg/kg bw) Imazalil 0.01/0.1/ (JMPR 2001) Maneb group (Dithiocarbamates) (EU 2005) 2 Mecarbam (JMPR 1986) Methamidophos 0.01/ (JMPR 2002) Methidathion 0.01/ (JMPR 1992) Mevinphos (JMPR 1996) Monocrotophos (JMPR 1993) Thiabendazole 0.01/0.2/ (EU 2001) Tolylfluanid (EU 2005) Triazophos (JMPR 2002) Vinclozolin (JMPR 1995) 1 each determined separately 2 dithiocarbamates was compared to the ADI of mancozeb Recalculation of for certain pesticides For dimethoate and omethoate, the residue definition for chronic risk assessment proposed in the EU was used: dimethoate plus 3 omethoate expressed as dimethoate. The residue levels of dithiocarbamates, expressed as CS 2, were converted to mancozeb in order to enable comparison with an ADI. Mancozeb was chosen since the compound is widely used. Results When the most conservative estimate (90 th percentile consumption and 95 th percentile residue level) was applied, the daily intake of pesticide from all commodities included in the study exceeded 1% of the ADI for 14 of the 22 pesticides. Dicofol and carbaryl reached the highest intake compared with the ADI, 11.9% and 6.0% respectively. When average residue level (negatives assigned the reporting level) and 90 th percentile consumption were used in the calculation, 9 of the pesticides exceeded 1% of the ADI. In the previous estimation in 2000, with the same pesticide/commodity combinations, 14 pesticides exceeded 1% of the ADI. Finally, if it was assumed that the pesticide was absent in the negative, none of the pesticides exceeded 1% of the ADI (Figure 8 and Table 14). Only the intake of mevinphos was zero since no of this pesticide were found in Livsmedelsverkets rapport nr 13/2006 National Food Administration, Sweden

30 13% 12% 11% 10% 9% 8% 11,9% a) average residue level, 90th percentile consumption, neg=0 b) average residue level, 90th percentile consumption, neg=rl c) 95th percentile residue level, 90th percentile consumption, neg=rl % of ADI 7% 6% 5% 4% 3% 2% 1% 6,0% 0% Azinphos-methyl Carbaryl Carbendazim Chlorpropham Dicofol Dimethoate Diquat Dithiocarbamates Endosulfan Imazalil Methamidophos Methidathion Monocrotophos Thiabendazole Figure 8. Pesticides with intake >1% of the ADI at the 90 th percentile consumption, 95 th percentile residue level and RL for negatives. National Food Administration, Sweden Livsmedelsverkets rapport nr 13/

31 Table 14. Total intake in % of the ADI at the 90 th percentile consumption. a b c Acephate Azinphos-methyl Carbaryl Carbendazim Chlormequat Chlorpropham Dicofol Dimethoate Diquat Dithiocarbamates Endosulfan Ethion Imazalil Mecarbam Methamidophos Methidathion Mevinphos Monocrotophos Thiabendazole Tolylfluanid Triazophos Vinclozolin a) average residue level, 90 th percentile consumption, negatives = 0 b) average residue level, 90 th percentile consumption, negatives = RL c) 95th percentile residue level, 90 th percentile consumption, negatives = RL Table 15 presents the intake in μg/person/day for the selected pesticides and also shows comparisons with previous estimations. The total intake (sum of all pesticides) based on the 90 th percentile consumption, reached 181 μg/person/day. This is an increase compared with the amount found in 2000 for the same pesticide/commodity combinations. An advantage in comparing the intake in μg/day instead of percentage of the ADI is that the figure is independent on changes in the ADIs and that comparisons could be performed for pesticides an established ADI. 30 Livsmedelsverkets rapport nr 13/2006 National Food Administration, Sweden