Study of Pesticide Residues in Agricultural Products towards the Positive List System

December 2005 305 17 7 8, Study of Pesticide Residues in Agricultural Products towards the Positive List System Yumi A@>N6B6,Naoki YDH=>D@6 and Keiko I8=>=6H=> (Hyogo Prefectural Institute of Public Health and Environmental Sciences: 2 1 29, Arata-cho, Hyogo-ku, Kobe 652 0032, Japan; Corresponding author) During a 3-year monitoring survey (April 2002 March 2005) of pesticide residues in agricultural products, 592 samples (324 domestic; 268 imported) collected in Hyogo prefecture, Japan were analyzed. The number of tested increased from 232 in FY 2002 to 323 in FY 2004. The purpose of the study was to clarify the residue status by accumulating information about detected frequently, to allow e#ective and e$cient regulation under the new Positive List legislation to be implemented in FY 2006. Overall, 47 of domestic and 61 of imported samples contained detectable residues and ca. 60 of positive samples contained multiple residues. The limit of quantitation was set at 0.01 mg/g and the limit of detection was 0.001 0.003 mg/ g. Most of the residues were present at low concentrations: 80 of the detections in samples excluding imported citrus fruits were 0.05 mg/g. More than 5 di#erent ( 0.01 mg/g) were detected simultaneously in 13 samples. The sum of the ratios of residues to MRLs was calculated as one of the indexes to represent the risk of multiple residues, and they exceeded 100 in 3 imported frozen vegetables; baby kidney bean, spinach, Welsh onion. Samples in violation of the Food Sanitation Law were not found in our survey, but 1.9 of the samples might be in conflict with the new Positive List legislation. (Received July 8, 2005) Key words: pesticide residue agricultural product the Positive List System simultaneous determination GC/MS LC/MS 1) 2006 500 1993 GC/MS 2) 4) 5) 10) 652 0032 2 1 29 1 27 p. 127 131 (2004.11), LC/MS GC/MS 100 1 2004 323 2002 2004 3 2005 5 31 1. 2002 4 2005 3 592 324 268, 119

306 2. 3. 2002 232 26 2003 291 35 2004 323 41 Table 1 2 240 23 GC/MS 83 18 LC/MS 4. Agilent 6890N 5973inert Agilent 1100 MSD (SL) 5. 9) ODS PSA GC/MS SCAN LC/MS SCAN 1 0.01 mg/g (S/N 3) 0.001 0.003 mg/g (Trace) 1. 2002 2004 3 592 2 Table 3 6 81 39 2 6), 10) Fig. 1 53 76 36 58 36 60 21 43 2. Table 4 5 Vol. 46, No. 6 (1) 2 0.02 mg/g 4 36 231 179 8 8 1 3 0.1 mg/g 0.01 mg/g 52 0.01 mg/g 0.05 mg/g 32 13 73 205 8 8 0.01 mg/g 0.05 mg/g 47 37 (2) 4 0.05 mg/g 15 46 49 21 119 162 0.1 mg/g 0.01 mg/g 0.05 mg/g 41 37 38 43 3 55 162 0.1 mg/g 35 0.5 mg/g 8 42 47

Organophosphorus pesticide Organochlorine pesticide N-Mmethylcarbamate Table 1. Llist of Pesticides Tested FYs 2002 2004 FYs 2003 2004 FY 2004 No. GC/MS main LC/MS main GC/MS main LC/MS main GC/MS main LC/MS main thiometon, tolclofosmethyl, triazophos quinalphos, terbufos, tetrachlorvinphos, profenofos, prothiofos, pyraclofos, phosphamidon, pirimiphosmethyl, phorate, phosalone, phosmet, parathion, parathionmethyl, phenthoate, monocrotophos, naled, omethoate, methacrifos, methidathion, isofenphos, isoxathion, malathion, fenthion, fonofos, fosthiazate, iprobenfos, etrimfos, fenitrothion, fensulfothion, -Z), edifenphos, ethion, ethoprophos, dichlorvos, dimethoate, dimethylvinphos(-e, cyanophos, demeton-s-methyl, diazinon, chlorpyrifosmethyl, cyanofenphos, chlorfenvinphos(-e, -Z), chlorpyrifos, cadusafos, carbophenothion, EPN, azinphosmethyl, butamifos, vamidothion phoxim, trichlorfon, methamidophos, Acephate, Anilofos, dichlofenthion, disulfoton, fenamiphos, isocarbophos, mecarbam, mevinphos, piperophos, propaphos, pyridaphenthion, sulprofos Dioxathion, isazofos Bensulide 69 BHC(a-, b-, g-, d-), DDT(p,p -, o,p -), aldrin, captafol, captan, chlordane, chlorobenzilate, dicofol, dieldrin, endosulfan(a-, b-), endrin, folpet, heptachlor, heptachlor epoxide (endo, exo), hexachlorobenzene, indanofan, methoxychlor, mirex, nonachlor, phthalide, quintozene Dichlobenil, dicloran, tecnazene, tetradifon 25 XMC, aldicarb, bendiocarb, carbaryl, carbofuran, ethiofencarb, fenobucarb, isoprocarb, methiocarb, methomyl, metolcarb, oxamyl, propoxur, terbucarb, xylylcarb Furathiocarb Thiodicarb 17 307 December 2005

Organonitrogen Pyrethroid Table 1. Continued FYs 2002 2004 FYs 2003 2004 FY 2004 No. GC/MS main LC/MS main GC/MS main LC/MS main GC/MS main LC/MS main EPTC, acibenzolar-s-methyl, alachlor, Acetamiprid, Ametryn, Bifenazate, atrazine, bifenox, bitertanol, bromacil, azoxystrobin, benalaxyl, chloridazon, buprofezin, butachlor, butylate, carpropamid, bromobutide, cumyluron, cafenstrole, chlomethoxyfen, clethodim, butafenacil, dymron, chlorfenapyr, chlornitrofen, clofentezine, carbetamide, fenpyroximate, chlorpropham, cyanazine, desmedipham, clomeprop, fentrazamide, cyhalofopbutyl, cyproconazole, ethoxyquin, dimepiperate, ferimzone (-E,-Z), cyprodinil, dichlofluanid, imazalil, dimethametryn, inabenfide, diclocymet, diethofencarb, imibenconazole, dithiopyr, nitenpyram, diethyltoluamide, difenoconazole, iprodione, etridiazole, oxadixyl, diflufenican, dimethenamid, mepanipyrim, fenbuconazole, oxaziclomefone, dimethomorph, diphenamid, methabenzthiazuron, fenothiocarb, oxpoconazole diphenylamine, esprocarb, ethychlozate, pencycuron, fenoxanil, fumarate, etobenzanid, etoxazole, famoxadone, prochloraz, fenpropimorph, phenmedipham, fenarimol, fenoxapropethyl, fipronil, propamocarb, fluacrypyrim, tepraloxydim, fludioxonil, flumioxazin, flusilazole, pymetrozine, indoxacarb-mp, thiacloprid flutolanil, furametpyr, hexaconazole, pyrazoxyfen, metalaxyl, kresoximmethyl, lenacil, mefenacet, tebufenozide, metominostrobin(-e, -Z), mepronil, metolachlor, metribuzin, thiabendazole, naproanilide, myclobutanil, nitrofen, paclobutrazol, tricyclazole oxabetrinil, penconazole, pendimethalin, pentoxazone, prometryn, pirimicarb, pretilachlor, procymidone, pyroquilon, propanil, propiconazole,propyzamide, quinoclamine, pyraflufenethyl, pyributicarb, pyridaben, thiamethoxam, pyrifenox(-e,-z), pyrimethanil, thiocyclam, pyrimidifen, pyriminobacmethyl(-e,-z), tolfenpyrad, pyriproxyfen, quizalofopethyl, simazine, trifloxystrobin simetryn, swep, tebuconazole, tebufenpyrad, terbacil, tetraconazole, thenylchlor, thifluzamide, thiobencarb, tolylfluanid, triadimefon, triadimenol, trichlamide, triflumizole, trifluralin, uniconazole P, vinclozolin Carfentrazone-ethyl, oxadiazon Amitraz, benzofenap, chlorfluazuron, chromafenozide, clothianidin, cyazofamid, cycloxydim, cymoxanil, diflubenzuron, dimethirimol, diuron, flufenoxuron, hexaflumuron, hexythiazox, imidacloprid, isouron, linuron, lufenuron, methoxyfenozide, probenazole, pyrazolate, teflubenzuron, triforine 175 Acrinathrin, allethrin, bifenthrin, bioresmethrin, cyfluthrin, cyhalothrin, cypermethrin, deltamethrin, ethofenprox, fenpropathrin, fenvalerate, flucythrinate, fluvalinate, halfenprox, imiprothrin, permethrin, phenothrin, pyrethrins, silafluofen, tefluthrin, tetramethrin, tralomethrin Cycloprothrin 23 308 Vol. 46, No. 6

Table 1. Continued FYs 2002 2004 FYs 2003 2004 FY 2004 No. GC/MS main LC/MS main GC/MS main LC/MS main GC/MS main LC/MS main Other Benfuresate, bromopropylate, cinmethylin, dimethipin, diphenyl, isoprothiolane, methoprene, phenothiol, piperonyl butoxide o-phenylphenol, propargite MCPB-ethyl MCPA-methyl Benzobicyclon 14 Total No. 192 40 43 16 5 27 323 Table 2. Llist of Pesticide Metabolites Tested FYs 2002 2004 FYs 2003 2004 FY 2004 No. GC/MS main LC/MS main GC/MS main LC/MS main GC/MS main LC/MS main Organophosphorus EPN oxon, demeton-s-methyl sulfone, diazinon oxon, fenitrothion oxon, isofenphos oxon, isoxathion oxon, malathion oxon, parathion oxon, parathionmethyl oxon, prothiofos oxon Vamidothion sulfone Disulfoton sulfone Demeton-S-methyl sulfoxide 13 Organochlorine p,p -DDE, p,p -DDD, endosulfan sulfate, dichlorobenzophenone (dicofol metabolite), oxychlordane, phthalimide (folpet methabolite), tetrahydrophthalimide (captan, captafol metabolite) 7 N-Methylcarbamate Aldicarb sulfone, aldicarb sulfoxide, ethiofencarb sulfone, ethiofencarb sulfoxide, methiocarb sulfone, methiocarb sulfoxide 7 3-Hydroxycarbofuran Organonitrogen Dichlofluanid metabolite, 2,4-dichloroaniline (imibenconazole metabolite), furametpyr metabolite, tolylfluanid metabolite, triflumizole metabolite Imazalil metabolite, imibenconazole desbenzyl, iprodione metabolite, mepanipyrim metabolite Oxpoconazole metabolite, thiacloprid-amide Amitraz metabolite, carbendazim, oxpoconazole formyl 14 Total No. 22 4 0 9 1 5 41 309 December 2005

310 Table 3. Number of Samples Tested and Containing Detectable Pesticide Residues during FYs 2002 2004 Sample group Tested No. Positive 1 Multi residues 2 No. No. Total 592 316 53 200 34 Domestic 324 152 47 95 29 Cereals 15 4 27 3 20 Beans 1 0 0 0 0 Vegetables 231 89 39 49 21 Fruits 73 59 81 43 59 Nuts & seeds 4 0 0 0 0 Imported 268 164 61 105 39 Cereals 6 5 83 1 17 Vegetables 46 21 46 9 20 Frozen vegetables 119 59 50 39 33 Citrus fruits 55 51 93 44 80 Other fruits 42 28 67 12 29 1 Samples containing 1 or more pesticide residues 0.001 mg/g 2 Samples containing multipesticide residues 0.001 mg/g 0.01 mg/g 0.05 mg/g 40 32 0.1 mg/g 0.5 mg/g 23 3. 0.01 mg/g Table 6 7 (1) 0.01 mg/g Vol. 46, No. 6 40 61 1 1 1 3 5 (2) 0.01 mg/g 50 56 80 19 5 2 1 1 1 2 4. Table 8 1 8) 11) 10 (ADI) 0.2 mg/kg/day 50 kg 40 g ADI Fig. 1. Detection rates of positive samples during FYs 1995 2004

December 2005 311 Table 4. Pesticide Residues Found in Domestic Agricultural Products (FYs 2002 2004) Pesticide Tested samples Residue ( mg/g) 0.01 0.05 0.1 0.5 1 1 Total detections Commodity Cereals Ferimzone 4 0 1 0 0 0 0 1 Unpolished rice Dichlorvos 15 1 0 0 0 0 0 1 Unpolished rice Isoprothiolane 15 1 0 0 0 0 0 1 Unpolished rice Phthalide 15 1 0 0 0 0 0 1 Unpolished rice Silafluofen 15 1 0 0 0 0 0 1 Unpolished rice Vegetables Procymidone 231 10 4 0 3 0 0 17 Cucumber, eggplant etc. Carbendazim 77 6 5 0 1 0 0 12 Lettuce, cucumber etc. Acetamiprid 231 5 3 1 0 1 0 10 Shirona, sweet pepper etc. Azoxystrobin 231 4 4 0 1 0 0 9 Tomato, cucumber etc. Methomyl 231 3 4 0 0 0 1 8 Babykidney bean etc. Ethofenprox 231 3 1 3 1 0 0 8 Green soybean, cucumber etc. Permethrin 231 3 3 1 1 0 0 8 Shirona, sweet pepper etc. Iprodione 231 5 2 0 1 0 0 8 Chinese cabbage, cucumber etc. Chlorfenapyr 231 3 4 0 0 0 0 7 Chinese cabbage, sweet pepper etc. Fenvalerate 231 2 3 1 0 0 0 6 Chinese cabbage, lettuce etc. Acephate 231 0 4 0 1 0 0 5 Carrot, lettuce etc. Oxadixyl 118 1 4 0 0 0 0 5 Cucumber, Chinese cabbage etc. Chlorotalonil 231 2 0 2 1 0 0 5 Asparagus, tomato etc. Methamidophos 231 3 0 2 0 0 0 5 Chinese cabbage, carrot etc. Metalaxyl 118 2 1 0 1 0 0 4 Cucumber, Chinese cabbage etc. Imidacloprid 77 3 1 0 0 0 0 4 Sweet pepper etc. Cypermethrin 231 1 2 0 0 0 0 3 Lettuce, Welsh onion Fruits Acetamiprid 73 6 12 0 2 0 0 20 Grape, apple etc. Kresoximmethyl 73 12 4 1 1 0 0 18 Grape, apple etc. Captan 73 2 6 1 2 0 0 11 Apple, Japanese pear etc. Cyprodinil 73 6 3 1 1 0 0 11 Grape, apple Carbendazim 21 7 3 1 0 0 0 11 Japanese persimmon, melon etc. Chlorpyrifos 73 5 5 0 0 0 0 10 Apple Fenpropathrin 73 3 2 3 1 0 0 9 Apple etc. Bromopropylate 73 2 2 4 0 0 0 8 Japanese pear, apple Iprodione 73 0 3 1 3 0 0 7 Grape, peach etc. Cyhalothrin 73 4 2 0 0 0 0 6 Apple Mepanipyrim 73 3 0 0 2 0 0 5 Grape etc. Carbaryl 73 3 2 0 0 0 0 5 Apple etc. Permethrin 73 0 3 0 1 0 0 4 Plum, Japanese persimmon etc. Fludioxonil 73 1 2 1 0 0 0 4 Grape Propargite 73 1 2 1 0 0 0 4 Apple Cypermethrin 73 1 3 0 0 0 0 4 Japanese persimmon Tebufenpyrad 73 3 0 0 1 0 0 4 Strawberry etc. Fenitrothion 73 3 1 0 0 0 0 4 Grape etc. Triflumizole 73 3 1 0 0 0 0 4 Grape etc. Azoxystrobin 73 1 2 0 0 0 0 3 Grape etc. Chlorfenapyr 73 1 2 0 0 0 0 3 Apple etc. Diazinon 73 2 1 0 0 0 0 3 Apple etc. Methamidophos 73 2 1 0 0 0 0 3 Fig etc.

312 Vol. 46, No. 6 Table 5. Pesticide Residues Found in Imported Agricultural Products (FYs 2002 2004) Pesticide Tested samples Residue ( mg/g) 0.01 0.05 0.1 0.5 1 1 Total detections Commodity Cereals Isoprothiolane 6 2 1 0 0 0 0 3 Polished rice Dichlorvos 6 0 1 0 0 0 0 1 Polished rice Vegetables Permethrin 46 1 0 2 0 0 0 3 Celery etc. Dicloran 22 0 0 0 1 1 0 2 Celery Omethoate 46 0 1 0 1 0 0 2 Okra, baby pea Carbendazim 15 0 2 0 0 0 0 2 Welsh onion, garlic sprout etc. Cypermethrin 46 0 2 0 0 0 0 2 Okra Propiconazole 46 0 2 0 0 0 0 2 Celery Frozen vegetables Cypermethrin 119 4 8 8 6 0 2 28 Spinach, komatsuna etc. Carbendazim 50 14 2 1 0 0 0 17 Baby kidney bean, komatsuna etc. Omethoate 119 4 7 1 1 0 0 13 Baby kidney bean, baby pea etc. Methamidophos 119 0 6 1 1 0 0 8 Broccoli, baby kidney bean etc. DDT 119 7 1 0 0 0 0 8 Baby kidney bean etc. Triadimenol 119 1 5 0 1 0 0 7 Baby pea, baby kidney bean etc. Chlorpyrifos 119 4 3 0 0 0 0 7 Komatsuna, baby kidney bean etc. Fenvalerate 119 1 3 1 1 0 0 6 Green soybean, Welsh onion etc. Methomyl 119 2 4 0 0 0 0 6 Baby kidney bean Dimethoate 119 3 3 0 0 0 0 6 Baby kidney bean, Welsh onion Cyproconazole 119 4 2 0 0 0 0 6 Baby kidney bean Endosulfan 119 0 4 0 0 0 0 4 Baby kidney bean, spinach etc. Chlorfenapyr 119 1 2 1 0 0 0 4 Green soybean etc. Fenpropathrin 119 1 1 0 1 0 0 3 Welsh onion, baby kidney bean Procymidone 119 0 1 0 1 0 0 2 Leek, spinach Dicofol 119 0 1 1 0 0 0 2 Baby kidney bean, green soybean Monocrotophos 119 0 2 0 0 0 0 2 Welsh onion, baby kidney bean Triazophos 119 0 2 0 0 0 0 2 Baby kidney bean, green soybean Citrus fruits Imazalil 55 1 3 2 7 10 20 43 Orange, grapefruit, lemon Thiabendazole 55 2 4 2 6 7 9 30 Orange, grapefruit, lemon Chlorpyrifos 55 3 7 7 6 0 0 23 Orange, grapefruit, lemon o-phenylphenol 55 4 3 0 6 1 1 15 Orange, grapefruit, lemon Methidathion 55 1 1 2 2 0 0 6 Orange, grapefruit, lemon Diphenylamine 55 0 3 1 0 0 0 4 Lemon Prothiofos 55 0 3 0 0 0 0 3 Grapefruit Diazinon 55 1 0 0 2 0 0 3 Orange, lemon Bromopropylate 55 2 0 0 1 0 0 3 Orange etc. Carbendazim 15 2 1 0 0 0 0 3 Lemon etc. Carbaryl 55 0 0 0 1 0 1 2 Lemon, orange Ethion 55 0 0 2 0 0 0 2 Grapefruit Azoxystrobin 55 0 2 0 0 0 0 2 Grapefruit Other fruits Chlorpyrifos 42 7 4 0 0 0 0 11 Banana etc. Triflumizole 42 0 1 0 3 0 0 4 Pineapple Iprodione 42 1 0 0 2 1 0 4 Banana, grape etc. Carbendazim 16 3 0 0 1 0 0 4 Banana etc. Myclobutanil 42 2 1 0 0 0 0 3 Cherry etc. Captan 42 0 0 0 2 0 0 2 Avocado, strawberry

December 2005 313 Table 6. Distribution of Multiple Pesticide Residues ( 0.01 mg/g) Detected on Domestic Samples Sample No. of detected residues Total positive samples Tested Group Commodity 1 2 3 4 5 6 No. samples Cereals Unpolished rice 1 0 0 0 0 0 1 50 2 Polished rice 0 0 0 0 0 0 0 0 2 Corn 1 0 0 0 0 0 1 13 8 Buckwheat 0 0 0 0 0 0 0 0 2 Wheat flour 0 0 0 0 0 0 0 0 1 Subtotal 2 0 0 0 0 0 2 13 15 Beans Soybean 0 0 0 0 0 0 0 0 1 Vegetables Green soybean 3 1 0 0 0 0 4 67 6 Cucumber 2 3 0 0 0 1 6 55 11 Lettuce 4 2 0 0 0 0 6 55 11 Tomato 5 3 0 0 0 0 8 47 17 Chinese cabbage 2 2 1 1 1 0 7 47 15 Sweet pepper 1 1 0 1 0 0 3 43 7 Welch onion 2 0 0 0 0 0 2 22 9 Eggplant 3 0 0 0 0 0 3 20 15 Cabbage 3 0 0 0 0 0 3 19 16 Carrot 0 2 0 0 0 0 2 15 13 Potato 1 0 0 0 0 0 1 8 13 Onion 0 0 0 0 0 0 0 0 18 Garden radish 0 0 0 0 0 0 0 0 10 Spinach 0 0 0 0 0 0 0 0 10 Komatsuna 0 0 0 0 0 0 0 0 9 Sweet potato 0 0 0 0 0 0 0 0 6 Broccoli 0 0 0 0 0 0 0 0 6 Garland chrysanthemum 1 0 0 0 0 0 1 25 4 Pumpkin 0 0 0 0 0 0 0 0 4 Taro 0 0 0 0 0 0 0 0 4 Baby kidney bean 1 0 0 0 0 0 1 33 3 Lotus root 0 0 0 0 0 0 0 0 3 Chingensai 1 0 0 0 0 0 1 50 2 Small green pepper 1 0 0 0 0 0 1 50 2 Broad bean 0 0 0 0 0 0 0 0 2 Burdock 0 0 0 0 0 0 0 0 2 Cauliflower 0 0 0 0 0 0 0 0 2 Celery 0 0 0 0 0 0 0 0 2 Nigauri 0 0 0 0 0 0 0 0 2 Asparagus 0 0 1 0 0 0 1 100 1 Ginger 1 0 0 0 0 0 1 100 1 Shirona 0 1 0 0 0 0 1 100 1 Aouri 0 0 0 0 0 0 0 0 1 Japanese mushroom 0 0 0 0 0 0 0 0 1 Santousai 0 0 0 0 0 0 0 0 1 Turnip 0 0 0 0 0 0 0 0 1 Subtotal 31 15 2 2 1 1 52 23 231 Fruits Grape 2 2 4 0 0 1 9 100 9 Japanese pear 5 2 0 0 0 0 7 88 8 Apple 2 1 5 2 1 2 13 87 15 Japanese persimmon 3 1 1 0 0 0 5 83 6 Fig 1 3 0 0 0 0 4 67 6 Peach 1 0 1 0 0 0 2 33 6 Watermelon 1 0 0 0 0 0 1 11 9 Melon 2 1 0 0 0 0 3 75 4 Mandarin orange 0 0 0 0 0 0 0 0 4 Strawberry 0 0 0 1 0 0 1 50 2 Loquat 0 0 0 0 0 0 0 0 2 Japanese plum 1 0 0 0 0 0 1 100 1 Summer orange 0 0 0 0 0 0 0 0 1 Subtotal 18 10 11 3 1 3 46 63 73 Nuts & seeds Chestnut 0 0 0 0 0 0 0 0 4 Total 51 25 13 5 2 4 100 31 324

314 Vol. 46, No. 6 Table 7. Distribution of Multiple Pesticide Residues ( 0.01 mg/g) Detected on Imported Samples Sample No. of detected residues Total positive samples Tested Group Commodity 1 2 3 4 5 6 No. samples Cereals Polished rice 2 0 0 0 0 0 2 40 5 Wheat flour 0 0 0 0 0 0 0 0 1 Subtotal 2 0 0 0 0 0 2 33 6 Vegetables Okra 2 3 0 0 0 0 5 83 6 Broccoli 2 0 0 0 0 0 2 17 12 Pumpkin 0 0 0 0 0 0 0 0 8 Burdock 1 0 0 0 0 0 1 33 3 Celery 0 0 0 0 2 0 2 100 2 Welsh onion 1 0 0 0 0 0 1 50 2 Sweet pepper 0 0 0 1 0 0 1 50 2 Asparagus 0 0 0 0 0 0 0 0 2 Japanese mushroom 0 0 0 0 0 0 0 0 2 Garlic 0 0 0 0 0 0 0 0 2 Garlic sprout 1 0 0 0 0 0 1 100 1 Baby pea 0 1 0 0 0 0 1 100 1 Guava tea 0 0 0 0 0 0 0 0 1 Baby snack pea 0 0 0 0 0 0 0 0 1 Onion 0 0 0 0 0 0 0 0 1 Subtotal 7 4 0 1 2 0 14 30 46 Frozen Green soybean 2 3 0 1 0 0 6 100 6 vegetables Baby pea 4 1 0 0 0 0 5 83 6 Baby kidney bean 4 1 6 0 0 1 12 67 18 Komatsuna 0 1 2 1 0 0 4 57 7 Spinach 4 0 1 1 0 0 6 55 11 Welsh onion 0 2 0 0 0 1 3 38 8 Okra 1 1 0 0 0 0 2 33 6 Chingensai 2 0 0 0 0 0 2 33 6 Broccoli 1 0 0 0 0 0 1 8 12 Taro 0 0 0 0 0 0 0 0 12 Pea 0 0 0 0 0 0 0 0 9 Asparagus 0 0 0 0 0 0 0 0 3 Broad bean 0 0 0 0 0 0 0 0 3 Sweet pepper 1 0 0 0 0 0 1 50 2 Pumpkin 0 0 0 0 0 0 0 0 2 Japanese mushroom 0 0 0 0 0 0 0 0 2 Lotus root 0 0 0 0 0 0 0 0 2 Leek 0 1 0 0 0 0 1 100 1 Corn 0 0 0 0 0 0 0 0 1 Garlic sprout 0 0 0 0 0 0 0 0 1 Mushroom 0 0 0 0 0 0 0 0 1 Subtotal 19 10 9 3 0 2 43 36 119 Citrus fruits Lemon 3 5 7 3 1 0 19 95 20 Orange 1 2 9 4 0 0 16 94 17 Grapefruit 6 5 1 1 1 1 15 83 18 Subtotal 10 12 17 8 2 1 50 91 55 Other fruits Banana 7 1 0 0 0 0 8 62 13 Pineapple 4 1 0 0 0 0 5 56 9 Avocado 2 0 0 0 0 0 2 40 5 Kiwi fruit 0 0 0 0 0 0 0 0 7 Grape 1 1 0 1 0 0 3 100 3 Cherry 2 0 0 0 0 0 2 67 3 Strawberry (frozen) 1 0 0 0 0 0 1 100 1 Melon 0 0 0 0 0 0 0 0 1 Subtotal 17 3 0 1 0 0 21 50 42 Total 55 29 26 13 4 3 130 49 268

December 2005 315 Table 8. Multiple Pesticide Residues in Agricultural Products Cucumber (domestic) (2004.6) 1 Chinese cabbage (domestic) (2002.10) Pesticide Residue MRL 2 ( ) 3 Pesticide Residue MRL ( ) Chlorfenapyr 0.01 1 1.0 Acephate 0.04 5.0 0.8 Metalaxyl 0.14 2 7.0 Methamidophos 0.07 Mepanipyrim 0.07 2 3.5 Chlorfenapyr 0.02 1 2.0 Procymidone 0.04 5 0.8 Fenvalerate 0.02 3.0 0.7 Oxadixyl 0.04 5 0.8 Famoxadone 0.04 1 4.0 Cabendazim 0.03 3 1.0 Imidacloprid Tr. 4 1 Total (Residue/MRL 14.1 Total (Residue/MRL 7.5 Grape (domestic) (2002.7) Apple (domestic) (2003.11) Pesticide Residue MRL ( ) Pesticide Residue MRL ( ) Acetamiprid 0.16 5 3.2 Chlorpyrifos 0.04 1.0 4.0 Fenitrothion 0.02 0.2 10.0 Prothiofos Tr. 0.3 Permethrin 0.01 5.0 0.2 Fenpropathrin 0.09 5 1.8 Cyprodinil 0.17 5 3.4 Cyhalothrin 0.01 0.4 2.5 Folpet 0.01 2 0.5 Acetamiprid 0.02 5 0.4 Fludioxonil 0.09 5 1.8 Cyprodinil 0.01 5 0.2 Mepanipyrim 0.26 15 1.7 Kresoximmethyl 0.02 5 0.4 Triflumizole 0.01 2.0 0.5 Pyrimethanil Tr. 10 Total (Residue/MRL 21.3 Total (Residue/MRL 9.3 Celery (America) (2005.1) Paprika (sweet pepper) (Korea) (2004.7) Pesticide Residue MRL ( ) Pesticide Residue MRL ( ) Acephate 0.01 10 0.1 Chlorfenapyr 0.07 1 7.0 Methamidophos Tr. Pyridaben Tr. 3.0 Permethrin 0.06 2.0 3.0 Oxadixyl 0.14 5 2.8 DDT Tr. 0.2 Imidacloprid 0.08 5 1.6 Oxamyl Tr. 5 Azoxystrobin 0.01 Dicloran 0.31 5.0 6.2 Procymidone Tr. 5 Propiconazole 0.02 5.0 0.4 Azoxystrobin Tr. 5 Linuron Tr. 0.2 Total (Residue/MRL 9.7 Total (Residue/MRL 11.4 Spinach, frozen (China) (2002.9) Komatsuna, frozen (China) (2004.12) Pesticide Residue MRL ( ) Pesticide Residue MRL ( ) Chlorpyrifos 0.01 0.01 100.0 Chlorpyrifos 0.02 1 2.0 Methamidophos 0.01 Fipronil 0.27 Parathionmethyl Tr. 1.0 Acetamiprid 0.03 5 0.6 DDT Tr. 0.2 DDT Tr. 0.2 Cypermethrin 1.93 2.0 96.5 Cyhalothrin 0.02 0.5 4.0 Fenvalerate 0.04 0.5 8.0 Cabendazim Tr. 3 Total (Residue/MRL 204.5 Total (Residue/MRL 6.6

316 Vol. 46, No. 6 Table 8. Continued Baby kidney bean, frozen (China) (2002.7) Welsh onion, frozen (China) (2004.2) Pesticide Residue MRL ( ) Pesticide Residue MRL ( ) Chlorpyrifos 0.01 0.2 5.0 Monocrotophos 0.04 0.05 80.0 Dimethoate 0.03 1 3.0 Dimethoate 0.02 1 2.0 Omethoate 0.11 Omethoate Tr. Methamidophos 0.06 Isocarbophos 0.01 Monocrotophos 0.04 0.05 80.0 Endosulfan 0.01 0.5 2.0 DDT 0.01 0.2 5.0 Cypermethrin 0.40 5.0 8.0 Dicofol 0.07 2 3.5 Fenvalerate 0.08 0.50 16.0 Buprofezin Tr. Fenpropathrin 0.15 Pyridaben Tr. 2.0 Carbofuran Tr. Methomyl 0.03 0.5 6.0 Triadimenol Tr. Isoprocarb Tr. Paclobutrazol 0.19 Cypermethrin 0.04 0.5 8.0 Fenvalerate 0.03 1.0 3.0 Fenpropathrin 0.02 Propargite 0.01 Triadimenol 0.01 1 1.0 Total (Residue/MRL 114.5 Total (Residue/MRL 108.0 Green soybean, frozen (China) 2003.7 Grape (Chile) 2002.5 Pesticide Residue MRL ( ) Pesticide Residue MRL ( ) Cypermethrin 0.34 5.0 6.8 Methomyl 0.15 1 15.0 Fenvalerate 0.16 1.0 16.0 Iprodione 0.31 25 1.2 Dicofol 0.03 2 1.5 Cyprodinil 0.17 5 3.4 Chlorfenapyr 0.01 Fludioxonil 0.04 5 0.8 DDT Tr. 2.0 Dichlorvos Tr. 0.5 Total (Residue/MRL 24.3 Total (Residue/MRL 20.4 Grapefruit (America) 2002.11 Lemon (Chile) 2003.10 Pesticide Residue MRL ( ) Pesticide Residue MRL ( ) 1 2 3 4 Imazalil 0.76 5.0 15.2 Imazalil 0.86 5.0 17.2 Imazalil met. 0.14 Imazalil met. 0.51 Thiabendazole 0.17 10 1.7 Thiabendazole 1.08 10 10.8 o-phenylphenol 2.46 10 24.6 Diphenylamine 0.02 Azoxystrobin 0.05 Metalaxyl 0.04 1 4.0 Chlorpyrifos 0.04 0.3 13.3 Chlorpyrifos 0.01 0.3 3.3 Ethion 0.08 0.3 26.7 Total (Residue/MRL 81.5 Total (Residue/MRL 35.3 Date of test year, month Standards for Withholding Registration of Pesticides on Crop Residues are represented in Italic letter, and others are Pesticide Residues Standards ( mg/g). Residue (mg/g) / MRL (mg/g) ( ) Tr. indicates trace level residue (0.001 0.01 mg/g) was detected.

December 2005 317 Table 9. Pesticide Residues Suggestive of Unregistered Application Commodity (Date of test year, month) Pesticide Residue (mg/g) MRL 1 Carrot (domestic) (2003. 6) Acephate 0.15 Methamidophos 0.06 Corn (domestic) (2003. 7) Acephate Tr. 2 0.5 Methamidophos 0.02 Fig (domestic) (2003. 8) Acephate Tr. 1.0 Methamidophos 0.03 0.1 Chingensai (domestic) (2005. 1) Oxadixyl 0.02 Garland chrysanthemum (domestic) (2005. 1) Carbendazim 0.02 Baby kidney bean (domestic) (2002. 7) Methomyl 1.0 Tomato (domestic) (2003. 6) Methomyl 0.04 1 Pesticide Residues Standards (mg/g) in Food Sanitation Law 2 Tr. indicates trace level residue (0.001 0.01 mg/g) was detected. Table 10. Pesticide Residues PotentiallyViolating the New Positive List Legislation Commodity (Date of test year, month) Pesticide Residue (mg/g) MRL 1 Carrot (domestic) (2003. 6) Acephate 0.15 0.01 2 Methamidophos 0.06 0.01 Orange (New Zealand) (2002.11) Diazinon 0.20 0.1 Lemon (Chile) (2003.10) Diphenylamine 0.07 0.05 Broccoli (America) (2003. 8) Oxaziclomefon 0.04 0.02 Okra (Thailand) (2002.12) EPN 0.14 0.01 2 Baby kidney bean, frozen (Thailand) (2004. 9) Cyproconazole 0.02 0.01 2 Baby kidney bean, frozen (China) (2002. 7) Fenpropathrin 0.02 0.01 2 Breen Soybean, frozen (Taiwan) (2003. 6) Chlorfenapyr 0.03 0.01 2 Breen Soybean, frozen (China) (2003. 7) Chlorfenapyr 0.06 0.01 2 Komatsuna, frozen (China) (2004.12) Fipronil 0.27 0.002 Welsh onion, frozen (China) (2004. 2) Paclobutrazol 0.19 0.01 2 Fenpropathrin 0.15 0.01 2 1 2 The Final Draft of Provisional Maximum Residue Limits (mg/g) in Food Sanitation Law The uniform level set as the level having no potential to cause damage to human health 0.002 mg/g ADI 0.6 mg/kg/day 0.05 mg/g 100 100 5. 1 0.5 mg/g 1.0 mg/g Table 9 2004 2 2005 3 Table 9 6. (0.01 mg/g) 2005 5 31 11 Table 10 1.9 2 2004 8 20 2.5 12) 2 2002 4 2005 3 592 232 323

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