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Appendix A. Supplementary DataArticle Title: Heavy Metal and Pesticide Content in Commonly Prescribed IndividualRaw Chinese Herbal MedicinesAuthor List:Eric S. J. HARRISShugeng CAOBruce A. LITTLEFIELDJane A. CRAYCROFTRobert SCHOLTENTed KAPTCHUKYanling FUWenquan WANGYong LIUHubiao CHENZhongzhen ZHAOJon CLARDYAlan D. WOOLFDavid M. EISENBERGSupplementary Data, Table of Contents:Page #Contents1Title Page2–3Supplementary Data, Table S1. List of plant speciesincluded in the study (N 126).4Supplementary Data, Table S2. List of all pesticideresidues screened (N 162).5–7Supplementary Data, Table S3. Reference values forpesticides and heavy metals.8Supplementary Data, Table S4. Summary of pesticideresidues detected (LOD 10–50 ppb; total of 162 pesticidesscreened) in raw Chinese Herbal Medicines (Total N 294).9References1
Supplementary Data, Table S1. List of plant species included in the study (N 126).Scientific Name (as listed in the Chinese Pharmacopoeia (CPC 2005))Acanthopanax senticosus (Rupr. ex Maxim.) HarmsAchyranthes bidentata Bl.Acorus tatarinowii SchottAgrimonia pilosa Ledeb.Akebia quinata (Thunb.) Decne.Alisma orientalis (Sam.) Juzep.Alpinia officinarum HanceAlpinia oxyphylla Miq.Amomum villosum Lour.Andrographis paniculata (Burm. f.) NeesApocynum venetum L.Arctium lappa L.Areca catechu L.Artemisia annua L.Artemisia argyi Lévl. et VantArtemisia capillaris Thunb.Asarum heterotropoides var. mandshuricum (Maxim.) Kitag.Aster tataricus L. f.Astragalus membranaceus var. mongholicus (Bge.) HsiaoAtractylodes macrocephala Koidz.Belamcanda chinensis (L.) DC.Brassica juncea (L.) Czern. et Coss.Brucea javanica (L.) Merr.Bupleurum chinense DC.Cassia tora L.Celosia cristata L.Chaenomeles speciosa (Sweet) NakaiChrysanthemum indicum L.Chrysanthemum morifolium Ramat.Citrus aurantium L.Citrus medica var. sarcodactylis SwingleCitrus reticulata BlancoClematis chinensis OsbeckCodonopsis pilosula (Franch.) Nannf.Coix lacryma-jobi L.Coptis chinensis Franch.Cornus officinalis Sieb. et Zucc.Corydalis yanhusuo W. T. WangCynanchum atratum Bge.Cynanchum paniculatum (Bge.) Kitag.Dianthus chinensis L.Dictamnus dasycarpus Turcz.Dimocarpus longan Lour.Dioscorea nipponica MakinoDioscorea opposita Thunb.Dipsacus asperoides C.Y. Cheng et T.M.AiDolichos lablab L.Echinops latifolius TauschEpimedium brevicornum Maxim.Eriobotrya japonica (Thunb.) Lindl.Evodia rutaecarpa (Juss.) Benth.Forsythia suspensa (Thunb.) VahlFritillaria cirrhosa D. DonGanoderma lucidum (Curtis) Karst.Gardenia jasminoides EllisGentiana macrophylla Pall.Ginkgo biloba L.Glehnia littoralis F. Schmidt ex Miq.Glycyrrhiza uralensis Fisch.Hedyotis diffusa Willd.Houttuynia cordata Thunb.Illicium verum Hook. f.Imperata cylindrica var. major (Nees) C. E. Hubb.Inula japonica Thunb.Isatis indigotica Fort.Juncus effusus L.Kaempferia galanga L.Kochia scoparia (L.) Schrad.Pin Yin NameCi Wu JiaNiu XiShi Chang PuXian He CaoMu TongZe XieGao Liang JiangYi ZhiSha RenChuan Xin LianLuo Bu Ma YeNiu Bang ZiDa Fu PiQing HaoAi YeYin ChenXi XinZi WanHuang QiBai ZhuShe GanJie ZiYa Dan ZiChai HuJue Ming ZiJi Guan HuaMu GuaYe Ju HuaJu HuaZhi QiaoFo ShouChen PiWei Ling XianDang ShenYi Yi RenHuang LianShan Zhu YuYan Hu SuoBai WeiXu Chang QingQu MaiBai Xian PiLong Yan RouChuan Shan LongShan YaoXu DuanBai Bian DouYu Zhou Lou LuYin Yang HuoPi Pa YeWu Zhu YuLian QiaoChuan Bei MuLing ZhiZhi ZiQin JiaoBai GuoBei Sha ShenGan CaoBai Hua She She CaoYu Xing CaoBa Jiao Hui XiangBai Mao GenJin Fei CaoBan Lan GenDeng Xin CaoShan NaiDi Fu ZiMedicinal PartRoot, Rhizome & StemRootRhizomeLeaf & StemStemTuberRhizomeFruitFruitLeaf & StemLeafFruitFruitLeaf & StemLeafLeaf & StemRoot & RhizomeRoot & uitFlowerFlowerFruitFruitFruitRoot & RhizomeRootSeedRhizomeFruitTuberRoot & RhizomeRoot & RhizomeLeaf & StemRootFruitRhizomeRhizomeRootSeedRootLeaf & StemLeafFruitFruitBulbFungusFruitRootSeedRootRoot & RhizomeLeaf & StemLeaf & StemFruitRhizomeLeaf & StemRootStemRhizomeFruit2
Scientific Name (as listed in the Chinese Pharmacopoeia (CPC 2005))Leonurus heterophyllus Sweet.Ligusticum chuanxiong Hort.Ligustrum lucidum Ait.Lindera aggregata (Sims)KostermLobelia chinensis Lour.Lonicera japonica Thunb.Lophatherum gracile Brongn.Lycium barbarum L.Lycopus lucidus var. hirtus RegelMelia toosendan Sieb. et Zucc.Menispermum dauricum DC.Mentha haplocalyx Briq.Momordica cochinchinensis (Lour.) Spreng.Momordica grosvenori SwingleMorus alba L.Paeonia lactiflora Pall.Paeonia suffruticosa Andr.Paeonia veitchii Lynch.Panax ginseng C.A. Mey.Panax notoginseng (Burk.) F.H. ChenPerilla frutescens (L.) Britt.Phragmites communis Trin.Piper nigrum L.Platycodon grandiflorum (Jacqui) A. DC.Pogostemon cablin (Blanco) Benth.Polygala tenuifolia Willd.Polygonum aviculare L.Polygonum cuspidatum Sieb. et Zucc.Polygonum multiflorum Thunb.Poria cocos (Schw.) WolfPortulaca oleracea L.Prunus armeniaca var. ansu Maxim.Pseudostellaria heterophylla (Miq.) Pax ex Pax et Hoffm.Pueraria lobata (Willd.) OhwiRehmannia glutinosa Libosch.Rheum palmatum L.Rosa laevigata Michx.Rosa rugosa Thunb.Rubia cordifolia L.Salvia miltiorrhiza Bge.Saposhnikovia divaricata (Turcz.) Schischk.Sarcandra glabra (Thunb.) NakaiSchisandra chinensis (Turcz.) Baill.Scutellaria baicalensis GeorgiSiegesbeckia orientalis L.Silybum marianum (L.) Gaertn.Sophora flavescens Ait.Sparganium stoloniferum Buch.-Ham.Stellaria dichotoma var. lanceolata Bge.Trachelospermum jasminoides (Lindl.) Lem.Tribulus terrestris L.Tussilago farfara L.Uncaria rhynchophylla (Miq.) Jacks.Verbena officinalis L.Xanthium sibiricum Patr.Zanthoxylum bungeanum Maxim.Ziziphus jujuba var. inermis (Bunge) RehdZiziphus jujuba var. spinosa (Bunge) Hu et H. F. ChouPin Yin NameYi Mu CaoChuan XiongNu Zhen ZiWu YaoBan Bian LianJin Yin HuaDan Zhu YeGou Qi ZiZe LanChuan Lian ZiBei Dou GenBo HeMu Bie ZiLuo Han GuoSang YeBai ShaoMu Dan PiChi ShaoRen ShenSan QiZi Su ZiLu GenHu JiaoJie GengGuang Huo XiangYuan ZhiBian XuHu ZhangHe Shou WuFu LingMa Chi XianKu Xing RenTai Zi ShenGe GenDi HuangDa HuangJin Ying ZiMei Gui HuaQian CaoDan ShenFang FengZhong Jie FengWu Wei ZiHuang QinXi Xian CaoShui Fei JiKu ShenSan LengYin Chai HuLuo Shi TengJi LiKuan Dong HuaGou TengMa Bian CaoCang Er ZiHua JiaoDa ZaoSuan Zao RenMedicinal PartLeaf & StemRhizomeFruitTuberWhole PlantFlowerLeaf & StemFruitLeaf & StemFruitRhizomeLeaf & ruitRootLeaf & StemRootLeaf & StemRoot & RhizomeTuberFungusLeaf & StemSeedTuberRootTuberRoot & RhizomeFruitFlowerRoot & RhizomeRoot & RhizomeRootWhole PlantFruitRootLeaf & StemFruitRootRhizomeRootLeaf & StemFruitFlowerStemLeaf & StemFruitFruitFruitSeed3
Supplementary Data, Table S2. List of all pesticide residues screened (N 162).Pesticide Name3-HydroxycarbofuranAcetochlorAlachlorAldicarb (temik)Aldicarb sulfoneAldicarb AtrazineBendiocarbBenfluralinBHC, alphaBHC, betaBHC, ryl (Sevin)Carbofuran (Furadan)CarbophenothionChlordane, cisChlordane, technicalChlordane, thrinCyprodinilDCPADDE, o,p'DDE, p,p'DDT, o,p'DDT, nitramineDioxacarbDiphenylamineEndosulfan IEndosulfan IIPesticide NameEndosulfan SulfateEndrinEndrin chlorHeptachlor homyl (Lannate)MethoprotryneMethoxychlor, o,p'Methoxychlor, obutanilNapropamideNitralinNitrofenNonachlor, cisNonachlor, transOctachlor PermethrinsPerthanePesticide tepTDE, o,p'TDE, p, p'TDE, trahydrophthalimide in4
Supplementary Data, Table S3. Reference values for pesticides and heavy metals.ContaminantArsenicArsenicTypeHeavy MetalHeavy MetalArsenicHeavy MetalCadmiumCadmiumHeavy MetalHeavy MetalCadmiumHeavy MetalChromiumHeavy MetalChromiumHeavy MetalChromiumHeavy MetalLeadHeavy MetalMercuryHeavy MetalMercuryHeavy MetalMercuryHeavy sticideCarbofuran deDDT, p,p'DDT, p,p'PesticidePesticideRfD, PAD, or MRLSource of RfD/MRL(mg/kg body wt/day)ATSDR Acute, oral exposure0.005ATSDR Chronic, oral exposure0.0003EPA-IRIS for Inorganic Arsenic,0.0003Chronic Oral ExposureATSDR Chronic Oral Exposure0.0001ATSDR Int. Oral Exposure0.0005EPA-IRIS for Chronic Oral0.001Exposure in FoodATSDR Chronic Oral Exposure0.001(for Cr VI)ATSDR Int. Oral Exposure (for Cr0.005VI)EPA-IRIS Chronic Oral Exposure0.003(for Cr VI)JECFA (based on the provisionaltolerable weekly intake [PTWI] for0.0036lead of 25 µg/kg body wt perweek)ATSDR Chronic Oral Exposure to0.0003Methyl MercuryATSDR Int. Oral Exposure to0.002Mercuric ChlorideJECFA (based on the ProvisionalTolerable Weekly Intake [PTWI]0.00057for inorganic mercury of 4 µg/kgbody wt per week)EPA ISTEP PAD, Acute Dietary,1.5Females 13-49EPA ISTEP PAD, Chronic Dietary,0.01General PopulationATSDR Acute MRL0.01ATSDR Int. MRL0.003EPA ISTEP PAD, Acute Dietary,0.01Females 13-49EPA ISTEP PAD, Chronic Dietary,0.0018General PopulationEPA ISTEP PAD, Acute Dietary,0.0002General PopulationATSDR Acute MRL0.003ATSDR Chronic MRL0.001EPA ISTEP PAD, Acute Dietary,0.0005General PopulationEPA ISTEP PAD, Chronic Dietary,0.00003General PopulationATSDR Acute MRL0.0005ATSDR Chronic MRL0.00055
myl (Lannate)PesticideMethomyl (Lannate)PesticideMyclobutanilPesticideRfD, PAD, or MRLSource of RfD/MRL(mg/kg body wt/day)EPA ISTEP PAD, Chronic Dietary,0.1General PopulationATSDR Chronic MRL0.002ATSDR Int. MRL0.005EPA ISTEP PAD, Acute Dietary,0.051General PopulationEPA ISTEP PAD, Chronic Dietary,0.006General PopulationATSDR Chronic MRL0.0003ATSDR Int. MRL0.002EPA ISTEP PAD, Acute Dietary,0.0018General PopulationEPA ISTEP PAD, Chronic Dietary,0.0018General PopulationEPA ISTEP PAD, Acute Dietary,0.06General PopulationEPA ISTEP PAD, Chronic Dietary,0.025General PopulationEPA ISTEP PAD, Acute Dietary,0.0018General PopulationEPA ISTEP PAD, Chronic Dietary,0.0018General PopulationEPA ISTEP PAD, Acute Dietary,0.025General PopulationEPA ISTEP PAD, Chronic Dietary,0.0002General PopulationEPA ISTEP PAD, Acute Dietary,0.02Females 13-49EPA ISTEP PAD, Chronic Dietary,0.06General PopulationEPA ISTEP PAD, Acute Dietary,0.02General PopulationEPA ISTEP PAD, Chronic Dietary,0.0016General PopulationATSDR Chronic MRL0.02ATSDR Int. MRL0.02EPA ISTEP PAD, Acute Dietary,0.076General PopulationEPA ISTEP PAD, Chronic Dietary,0.071General PopulationEPA ISTEP PAD, Acute Dietary,0.02General PopulationEPA ISTEP PAD, Chronic Dietary,0.008General PopulationEPA ISTEP PAD, Acute Dietary,0.6Females 13-496
sticideTrifluralinPesticideRfD, PAD, or MRLSource of RfD/MRL(mg/kg body wt/day)EPA ISTEP PAD, Chronic Dietary,0.025General PopulationATSDR Chronic MRL0.0003ATSDR Int. MRL0.0007EPA ISTEP PAD, Acute Dietary,0.00011General PopulationEPA ISTEP PAD, Chronic Dietary,0.00002General PopulationATSDR Acute MRL0.3ATSDR Int. MRL0.2EPA ISTEP PAD, Acute Dietary,0.25General PopulationEPA ISTEP PAD, Chronic Dietary,0.25General PopulationEPA ISTEP PAD, Acute Dietary,0.035Females 13-49EPA ISTEP PAD, Chronic Dietary,0.001General PopulationEPA ISTEP PAD, Acute Dietary,0.0003General PopulationEPA ISTEP PAD, Chronic Dietary,0.00005General PopulationEPA ISTEP PAD, Acute Dietary,1Females 13-49EPA ISTEP PAD, Chronic Dietary,0.024General PopulationATSDR Agency for Toxic Substances and Disease Registry (ATSDR, 2010)EPA-IRIS Environmental Protection Agency Integrated Risk Information System (US EPA, 2010)EPA-ISTEP Environmental Protection Agency (EPA) Office of Pesticide Programs ISTEP ToxicologyEndpoint Selection Database (David J. Miller, Chief, Chemistry & Exposure Branch, Office of PesticidePrograms, EPA, email communication, April 2010)JECFA-PTWI Joint FAO/WHO Expert Committee On Food Additives, Provisional Tolerable Weekly Intake(Pb: JECFA, 2000; Hg: JECFA, 2010)RfD Reference DosePAD Population Adjusted DoseMRL Minimal Risk Level (ATSDR, 2010)7
Supplementary Data, Table S4. Summary of pesticide residues detected (LOD 10–50 ppb; total of 162 pesticides screened) in raw Chinese Herbal Medicines (Total N 294).0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)65013670 (0%)68102955000144432460 (0%)5 (1.7%)13 (4.4%)18 (6.1%)37 (12.6%)0 (0%)0 (0%)2 (0.7%)2 (0.7%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)1 (0.3%)75 (25.5%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)1 (0.3%)1 (0.3%)50020*20*50050500100500 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)1 (0.3%)0 (0%)0 (0%)0 (0%)1 (0.3%)1 (0.3%)0 (0%)205051005 (1.7%)1 (0.3%)1 (0.3%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)1 (0.3%)0 (0%)0 (0%)0 (0%)1000500100500 (0%)0 (0%)1 (0.3%)1 (0.3%)1 (0.3%)100501001001001002 (0.7%)2 (0.7%)0 (0%)0 (0%)2 (0.7%)0 (0%)1 (0.3%)2 (0.7%)1 (0.3%)1 (0.3%)0 191810650 (0%)4 (1.4%)4 (1.4%)731496083874000 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)4 (1.4%)0 (0%)0 (0%)2 (0.7%)3 (1.0%)0 (0%)0 (0%)0 (0%)0 (0%)0 (0%)30850 (0%)471215111404923220253113011611013 (4.4%)1 (0.3%)1 (0.3%)0 (0%)1 (0.3%)0 (0%)0 (0%)3 (1.0%)60 (20.4%)4580442036478105211 (0.3%)1 (0.3%)1 (0.3%)2 (0.7%)1 (0.3%)0 (0%)0 (0%)66 (22.4%)68844534126505010050*50*50*505014 (4.8%)2432031594759# Samples Level# Samples 1% MRL(% samples in parentheses)Chronic Exposure0 (0%)0 (0%)(% samples in parentheses)# Samples 1% MRL(% samples in parentheses)Acute Exposure13# Samples 1% MRL(% samples in parentheses)Chronic Exposure11# Samples 1% MRL(% samples in parentheses)Acute Exposure12# Samples 1% PAD(% samples in parentheses)Chronic Exposure155166120# Samples 1% PAD(% samples in parentheses)Acute ExposureMaximum (ppb)302028# Samples 1% PAD(% samples in parentheses)Chronic ExposureMinimum (ppb)92934455Whole Herb Ingested# Samples 1% PAD(% samples in parentheses)Acute ExposureMedian (ppb)1 (0.3%)2 (0.7%)2 (0.7%)6 (2%)1 (0.3%)3 (1%)1 (0.3%)1 (0.3%)76 (25.9%)1 (0.3%)1 (0.3%)2 (0.7%)1 (0.3%)1 (0.3%)1 (0.3%)4 (1.4%)3 (1%)2 (0.7%)5 (1.7%)2 (0.7%)1 (0.3%)2 (0.7%)3 (1%)4 (1.4%)2 (0.7%)1 (0.3%)1 (0.3%)1 (0.3%)5 (1.7%)4 (1.4%)1 (0.3%)2 (0.7%)3 (1%)1 (0.3%)6 (2%)1 (0.3%)2 (0.7%)1 (0.3%)1 (0.3%)1 (0.3%)2 (0.7%)1 (0.3%)Value if N 1 (ppb)United StatesRegistration StatusRegisteredRegisteredNot Registered*Not Registered*Not Registered*Not RegisteredRegisteredNot RegisteredRegisteredNot Registered*Not Registered*Not Registered*RegisteredRegisteredNot RegisteredRegisteredNot RegisteredNot Not RegisteredNot Registered*RegisteredRegisteredRegisteredNot RegisteredNot RegisteredNot RegisteredNot Registered*Not Registered*Not Registered*RegisteredNot RegisteredNot RegisteredRegistered(% samples in parentheses)Pesticide NameAlachlorAtrazineBHC, alphaBHC, betaBHC, deltaBifenoxCarbofuran (Furadan)ChloropropylateChlorpyrifosDDE, p,p'DDT, o,p'DDT, p,p'DiphenylamineEndosulfan athionMethomyl (Lannate)MyclobutanilNonachlor, ethrinProcymidoneQuintozeneSulfotepTDE, o,p'TDE, p, p'TDE, anoxTrifluralin# Samples withDetectable PesticideHerb Taken as Soup/Tea,Assuming 10% LeachingComparison with ATSDR Minimal Risk Level (MRL) Comparison with Levels in EUPesticides Database (EUP, 2010) forvalues (ATSDR, 2010)Dried Herbal Infusions and FDAHerb Taken as Soup/Tea,Whole Herb Ingested Action Levels*Assuming 10% LeachingEU Maximum ResidueLevel or FDA ActionLevel* (ppb)General Summary Statistics for samples with detectableComparison with EPA-ISTEP PAD valueslevels0 (0%)0 (0%)0 (0%)1 (0.3%)20*20*20*100 (0%)0 (0%)0 (0%)0 (0%)10011*Pesticide is no longer registered for use in the United States, but the FDA has established an Action Level (US FDA, 2009).All calculations were done using the maximum daily dose of the herb (CPC, 2005) and assuming a body weight of 70 kg.8
ReferencesATSDR (Agency for Toxic Substances and Disease Registry) [Internet]. ATSDRMinimal Risk Levels for Hazardous Substances (MRLs). [cited 2010 Sept 16]. Availablefrom: http://www.atsdr.cdc.gov/mrls/index.htmlCPC (Chinese Pharmacopoeia Commission). Pharmacopoeia of the Peoples Republic ofChina: 2005. Beijing, China: People's Medical Publishing House; 2005.EUP (European Union Pharmacopoeia) [Internet]. European Union PharmacopoeiaPesticides Database. [cited 2010 Oct 10]. Available from:http://ec.europa.eu/sanco pesticides/public/index.cfmJECFA (Joint FAO/WHO Expert Committee on Food Additives). Evaluation of CertainFood Additives and Contaminants. WHO Technical Report Series No. 837. Geneva,Switzerland: WHO; 2000.JECFA (Joint Food and Agricultural Organization of the United Nations/World HealthOrganization Expert Committee on Food Additives). JECFA Seventy-second meetingRome, 16-25 February 2010. Geneva, Switzerland: WHO; 2010.US EPA (United States Environmental Protection Agency) [Internet]. Integrated RiskInformation System (IRIS). [cited 2010 Nov 17]. Available from: http://www.epa.gov/irisUS FDA (United States Food and Drug Administration) [Internet]. Pesticide Residues inFood and Feed - Enforcement Criteria (CPG Sec. 575.100). [updated 2009 Sept 12; cited2010 Oct 10]. Available mpliancepolicyguidancemanual/ucm123236.htm9
Oct 10, 2010 · Chai Hu Root Cassia tora L. Jue Ming Zi Seed Celosia cristata L. Ji Guan Hua Flower Chaenomeles speciosa (Sweet) Nakai Mu Gua Fruit Chrysanthemum indicum L. Ye Ju Hua Flower Chrysanthemum morifolium Ramat. Ju Hua Flower Citrus aurantium L. Zhi Qiao Fruit Citrus medica var. sarcodactylis Swi
