Skip to main content
Top
Published in: International Archives of Occupational and Environmental Health 1/2004

01-01-2004 | Short Communication

Current internal exposure to pesticides in children and adolescents in Germany: urinary levels of metabolites of pyrethroid and organophosphorus insecticides

Authors: Ursel Heudorf, Jürgen Angerer, Hans Drexler

Published in: International Archives of Occupational and Environmental Health | Issue 1/2004

Login to get access

Abstract

Aim

Pesticides are widely used throughout the world, in agriculture to protect crops and in public health to control diseases transmitted by vectors or intermediate hosts. After the prohibition of organochlorines such as DDT, today, mainly pyrethroids and organophosphorus insecticides are used. Whereas many studies have been published on background exposure of the population to organochlorines, data on internal exposure of the population to pyrethroids and organophosphorus insecticides are scarce. Here, we report on internal exposure of children and young people, in an urban area in Germany, to pyrethroids and organophosphorus acids, assessed by the analysis of urinary levels of their corresponding specific metabolites.

Methods

Approximately 673 children and adolescents took part in this voluntary investigation, including 331 children <6 years of age. Their parents stated that they and their children had never used pyrethroids or organophosphorus acids in their homes or for medical reasons. We analysed their spot urine samples for six metabolites of organophosphorus insecticides [dimethyl-phosphate (DMP), diethyl-phosphate (DEP), dimethyl-thiophosphate (DMTP), diethyl-thiophosphate (DETP), dimethyl-dithiophosphate (DMDTP) and diethyl-dithiophosphate (DEDTP)] and for four metabolites of pyrethroids [cis-3-(2,2-dibromo-vinyl)-2,2-dimethyl-cyclopropane carboxylic acid (Br2CA), cis-3-(2,2-dichloro-vinyl)-2,2-dimethyl-cyclopropane carboxylic acid (cis-Cl2-CA ), trans-3-(2,2-dichloro-vinyl)-2,2-dimethyl-cyclopropane carboxylic acid (trans-Cl2-CA) and 4-fluoro-3-phenoxy-benzoic acid (F-PBA)] using gas chromatographic methods with mass-selective detection. The limit of detection was 0.1–0.2 μg/l for pyrethroid metabolites and 1 μg/l for metabolites of organophosphorus acids; in DMP it was 5 μg/l.

Results

The 95th percentiles of the urinary metabolite concentrations were, in microgrammes per litre, DMP 158, DMTP 180, DMDTP 12, DEP 17, DETP 8, DEDTP <1; Br2CA 0.30, cis-Cl2-CA 0.44, trans-Cl2-CA 1.22, F-PBA 0.30. There were no correlations between urinary metabolite levels and the age of the children.

Conclusion

Current background levels of internal exposure to pyrethroids and organophosphorus insecticides in children and adolescents in Germany are shown. Exposure to these substances in the general population is thought to occur mainly via residues in the diet. The level of background internal pyrethroid exposure in the children is orders of magnitude lower than the corresponding acceptable daily intake (ADI) values published, but the level of internal organophosphate exposure may reach and even exceed ADI values. This observation demands further investigation.
Literature
go back to reference Angerer J, Hardt J (1997) Excretion of organophosphorus metabolites in the general population (in German). Arbeitsmed Sozialmed Umweltmed 32:470–477 Angerer J, Hardt J (1997) Excretion of organophosphorus metabolites in the general population (in German). Arbeitsmed Sozialmed Umweltmed 32:470–477
go back to reference Angerer J, Ritter A (1997) Determination of pyrethroid metabolites in human urine using solid-phase extraction and gas chromatography–mass-spectrometry. J Chromatogr 695:217–226 Angerer J, Ritter A (1997) Determination of pyrethroid metabolites in human urine using solid-phase extraction and gas chromatography–mass-spectrometry. J Chromatogr 695:217–226
go back to reference Aprea C, Sciarra G, Orsi D, Boccalon P, Sartorelli P, Sartorelli E (1996) Urinary excretion of alkylphosphates in the general population (Italy). Sci Tot Environ 177:37–41CrossRef Aprea C, Sciarra G, Orsi D, Boccalon P, Sartorelli P, Sartorelli E (1996) Urinary excretion of alkylphosphates in the general population (Italy). Sci Tot Environ 177:37–41CrossRef
go back to reference Aprea C, Sciarra G, Sartorelli P, Sartorelli E (1997) Biological monitoring of exposure to chlorpyrifos-methyl by assay of urinary alkylphosphates and 3,5,6-trichloro-2-pyridinol, J Toxicol Environ Health 50:581–594 Aprea C, Sciarra G, Sartorelli P, Sartorelli E (1997) Biological monitoring of exposure to chlorpyrifos-methyl by assay of urinary alkylphosphates and 3,5,6-trichloro-2-pyridinol, J Toxicol Environ Health 50:581–594
go back to reference Aprea C, Strambi M, Novelli MT, Lunghini L, Bozzi N (2000) Biologic monitoring of exposure to organophosphorus pesticides in 195 Italian children. Environ Health Perspect 108:521–525PubMed Aprea C, Strambi M, Novelli MT, Lunghini L, Bozzi N (2000) Biologic monitoring of exposure to organophosphorus pesticides in 195 Italian children. Environ Health Perspect 108:521–525PubMed
go back to reference Butte W, Walker G, Heinzow B (1998) Reference values for urinary concentrations of the metabolites of permethrin Cl2-CA (3-(2,2-dichlorvinyl)-2,2-dimethylcyclopropanecarboxylic acid) and 3-PBA (3-phenoxybenzoicacid) (in German). Umweltmed Forsch Prax 3:21–26 Butte W, Walker G, Heinzow B (1998) Reference values for urinary concentrations of the metabolites of permethrin Cl2-CA (3-(2,2-dichlorvinyl)-2,2-dimethylcyclopropanecarboxylic acid) and 3-PBA (3-phenoxybenzoicacid) (in German). Umweltmed Forsch Prax 3:21–26
go back to reference Byrne SL, Shurdut BA, Saunders DG (1998) Potential chlorpyrifos exposure to residents following standard crack and crevice treatment. Environ Health Perspect 106:725–731PubMed Byrne SL, Shurdut BA, Saunders DG (1998) Potential chlorpyrifos exposure to residents following standard crack and crevice treatment. Environ Health Perspect 106:725–731PubMed
go back to reference Davis DL, Ahmed AK (1998) Exposures from indoor spraying of chlorpyrifos pose greater health risks to children than currently estimated. Environ Health Perspect 106:299–301PubMed Davis DL, Ahmed AK (1998) Exposures from indoor spraying of chlorpyrifos pose greater health risks to children than currently estimated. Environ Health Perspect 106:299–301PubMed
go back to reference Department for Nature and Environment, Schleswig-Holstein (1997) Contamination in house yards and household dust in four regions of Schleswig-Holstein, Germany (in German). Ministry for Environment, Nature, and Forestry, Kiel, Germany Department for Nature and Environment, Schleswig-Holstein (1997) Contamination in house yards and household dust in four regions of Schleswig-Holstein, Germany (in German). Ministry for Environment, Nature, and Forestry, Kiel, Germany
go back to reference Friedrich C, Becker K, Hoffmann G, Hoffmann K, Krause C, Nöllke P, Schulz C, Schwabe R, Seiwert M (1998) Pyrethroids in household dust in the German population. Data from two representative studies in Germany (in German). Gesundheitswesen 60:95–101PubMed Friedrich C, Becker K, Hoffmann G, Hoffmann K, Krause C, Nöllke P, Schulz C, Schwabe R, Seiwert M (1998) Pyrethroids in household dust in the German population. Data from two representative studies in Germany (in German). Gesundheitswesen 60:95–101PubMed
go back to reference Gibson JE, Peterson RK, Shurdut BA (1998) Human exposure and risk from indoor use of chlorpyrifos. Environ Health Perspect 106:303–306PubMed Gibson JE, Peterson RK, Shurdut BA (1998) Human exposure and risk from indoor use of chlorpyrifos. Environ Health Perspect 106:303–306PubMed
go back to reference Griffin P, Mason H, Heywood K, Cocker J (1999) Oral and dermal absorption of chlorpyrifos: a human volunteer study. Occup Environ Med 56:10–13PubMed Griffin P, Mason H, Heywood K, Cocker J (1999) Oral and dermal absorption of chlorpyrifos: a human volunteer study. Occup Environ Med 56:10–13PubMed
go back to reference Gunderson EL (1995) FDA Total diet study, July 1986–April 1991. Dietary intakes of pesticides, selected elements and other chemicals. J AOAC Int 78:1353–1363PubMed Gunderson EL (1995) FDA Total diet study, July 1986–April 1991. Dietary intakes of pesticides, selected elements and other chemicals. J AOAC Int 78:1353–1363PubMed
go back to reference Gurunathan S, Robson M, Freeman N, Buckley B, Roy A, Meyer R, Bukowski J, Lioy PJ (1998) Accumulation of chlorpyrifos on residential surfaces and toys accessible to children. Environ Health Perspect 106:9–16PubMed Gurunathan S, Robson M, Freeman N, Buckley B, Roy A, Meyer R, Bukowski J, Lioy PJ (1998) Accumulation of chlorpyrifos on residential surfaces and toys accessible to children. Environ Health Perspect 106:9–16PubMed
go back to reference Hardt J, Angerer J (2000) Determination of dialkylphosphates in human urine using gas-chromatography–mass spectrometry. J Anal Toxicol 24:678–684PubMed Hardt J, Angerer J (2000) Determination of dialkylphosphates in human urine using gas-chromatography–mass spectrometry. J Anal Toxicol 24:678–684PubMed
go back to reference Hardt J, Heudorf U, Angerer J (1999) Exposure of the general population to pyrethroids (in German) Umweltmed Forsch Prax 4:54–55 Hardt J, Heudorf U, Angerer J (1999) Exposure of the general population to pyrethroids (in German) Umweltmed Forsch Prax 4:54–55
go back to reference Heudorf U (2000) High internal exposure to organophosphorus insecticides caused by extremely high consumption of fruit? Case report. (in German) Umweltmed Forsch Prax 5:189–191 Heudorf U (2000) High internal exposure to organophosphorus insecticides caused by extremely high consumption of fruit? Case report. (in German) Umweltmed Forsch Prax 5:189–191
go back to reference Heudorf U, Angerer J (2001a) Internal exposure to PAHs of children and adults living in homes with parquet flooring containing high levels of PAHs in parquet glue. Int Arch Occup Environ Med 74:91–101CrossRef Heudorf U, Angerer J (2001a) Internal exposure to PAHs of children and adults living in homes with parquet flooring containing high levels of PAHs in parquet glue. Int Arch Occup Environ Med 74:91–101CrossRef
go back to reference Heudorf U, Angerer J (2001b) Metabolites of organophosphorus insecticides in urine specimens from inhabitants of a residential area. Environ Res 86:80–87CrossRefPubMed Heudorf U, Angerer J (2001b) Metabolites of organophosphorus insecticides in urine specimens from inhabitants of a residential area. Environ Res 86:80–87CrossRefPubMed
go back to reference Heudorf U, Angerer J (2001c) Metabolites of pyrethroid insecticides in urine specimens: current exposure in an urban population in Germany. Environ Health Perspect 109:213–217PubMed Heudorf U, Angerer J (2001c) Metabolites of pyrethroid insecticides in urine specimens: current exposure in an urban population in Germany. Environ Health Perspect 109:213–217PubMed
go back to reference Hill, RH, Head SL, Baker M, Gregg M, Shealy DB, Bailey SL, Williams CC, Samplson EJ, Needham LL (1995) Pesticide residues in urine of adults living in the United States: reference range concentrations. Environ Res 71:99–108CrossRefPubMed Hill, RH, Head SL, Baker M, Gregg M, Shealy DB, Bailey SL, Williams CC, Samplson EJ, Needham LL (1995) Pesticide residues in urine of adults living in the United States: reference range concentrations. Environ Res 71:99–108CrossRefPubMed
go back to reference Joint meeting of the FAO panel of experts on pesticide residues in food and the environment and the WHO expert group on pesticide residues. Pesticide residues in food: 1963/64–1995 evaluations. Food and Agriculture Organization of the United Nations (FAO), Rome, 1964–1995 Joint meeting of the FAO panel of experts on pesticide residues in food and the environment and the WHO expert group on pesticide residues. Pesticide residues in food: 1963/64–1995 evaluations. Food and Agriculture Organization of the United Nations (FAO), Rome, 1964–1995
go back to reference Koch HM, Hardt J, Angerer J (2001) Biological monitoring of exposure of the general population to organophosphorus pesticides chlorpyrifos and chlorpyrifos-methyl by determination of their specific metabolite 3,5,6-trichloro-2-pyridinol. Int J Hyg Environ Health 204:175–180PubMed Koch HM, Hardt J, Angerer J (2001) Biological monitoring of exposure of the general population to organophosphorus pesticides chlorpyrifos and chlorpyrifos-methyl by determination of their specific metabolite 3,5,6-trichloro-2-pyridinol. Int J Hyg Environ Health 204:175–180PubMed
go back to reference Landrigan PJ, Claudio L, Markowitz SB, Berkowitz GS, Brenner BL, Romero H, Wetmur JG, Matte TD, Gore AC, Godbold JH, Wolff MS (1999) Pesticides and inner-city children: exposures, risks, and prevention. Environ Health Perspect 107: [Suppl 3]431–437 Landrigan PJ, Claudio L, Markowitz SB, Berkowitz GS, Brenner BL, Romero H, Wetmur JG, Matte TD, Gore AC, Godbold JH, Wolff MS (1999) Pesticides and inner-city children: exposures, risks, and prevention. Environ Health Perspect 107: [Suppl 3]431–437
go back to reference Lemus R, Abdelghani A (2000) Chlorpyrifos: an unwelcome pesticide in our homes. Rev Environ Health 15:421–433PubMed Lemus R, Abdelghani A (2000) Chlorpyrifos: an unwelcome pesticide in our homes. Rev Environ Health 15:421–433PubMed
go back to reference Leng G, Kühn K-H, Idel H (1997a) Biological monitoring of pyrethroids in blood and pyrethroid metabolites in urine: applications and limitations. Sci Tot Environ 199:173–181CrossRef Leng G, Kühn K-H, Idel H (1997a) Biological monitoring of pyrethroids in blood and pyrethroid metabolites in urine: applications and limitations. Sci Tot Environ 199:173–181CrossRef
go back to reference Leng G, Leng A, Kühn K-H, Lewalter J, Pauluhn J (1997b) Human dose–excretion studies with the pyrethroid insecticide cyfluthrin: urinary metabolite profile following inhalation. Xenobiotica 27:1272–1283CrossRef Leng G, Leng A, Kühn K-H, Lewalter J, Pauluhn J (1997b) Human dose–excretion studies with the pyrethroid insecticide cyfluthrin: urinary metabolite profile following inhalation. Xenobiotica 27:1272–1283CrossRef
go back to reference Leoni V, Caricchia AM, Comi R, Martini F, Rodolico S, Vitali M (1995) Risk assessment of organophosphorus pesticide dietary intake for the population of the city of Rome (Italy). Bull Environ Contam Toxicol 54:870–877PubMed Leoni V, Caricchia AM, Comi R, Martini F, Rodolico S, Vitali M (1995) Risk assessment of organophosphorus pesticide dietary intake for the population of the city of Rome (Italy). Bull Environ Contam Toxicol 54:870–877PubMed
go back to reference Lu Ch, Fenske RA (1999) Dermal transfer of chlorpyrifos residues from residential surfaces: comparison of hand press, hand drag, wipe, and polyurethane foam roller measurements after broadcast and aerosol pesticide applications. Environ Health Perspect 107:463–467 Lu Ch, Fenske RA (1999) Dermal transfer of chlorpyrifos residues from residential surfaces: comparison of hand press, hand drag, wipe, and polyurethane foam roller measurements after broadcast and aerosol pesticide applications. Environ Health Perspect 107:463–467
go back to reference Macintosh DL, Spengler JD, Özkaynak H, Tsai L, Ryan B (1996) Dietary exposures to selected metals and pesticides. Environ Health Perspect 101:202–209 Macintosh DL, Spengler JD, Özkaynak H, Tsai L, Ryan B (1996) Dietary exposures to selected metals and pesticides. Environ Health Perspect 101:202–209
go back to reference Oglobline AN, Elimelakh H, Tattam B, Geyer R, O’Donnell GE, Holder G (2001) Negative ion chemical ionization GC/MS-MS analysis of dialkylphosphate metabolites of organophosphate pesticides in urine of non-occupationally exposed subjects. Analyst 126:1037–1041CrossRefPubMed Oglobline AN, Elimelakh H, Tattam B, Geyer R, O’Donnell GE, Holder G (2001) Negative ion chemical ionization GC/MS-MS analysis of dialkylphosphate metabolites of organophosphate pesticides in urine of non-occupationally exposed subjects. Analyst 126:1037–1041CrossRefPubMed
go back to reference Penttilä PL, Siivinen K (1996) Control and intake of pesticide residues during 1981–1993 in Finland. Food Addit Contam 13:609–622PubMed Penttilä PL, Siivinen K (1996) Control and intake of pesticide residues during 1981–1993 in Finland. Food Addit Contam 13:609–622PubMed
go back to reference Pöhner A, Simrock S, Thumulla J, Weber S, Wirner T (1997) Background contamination in household dust in private homes with semi- and nonvolatile organic compounds (in German). Analyse und Bewertung von Umweltschadstoffen (AnBUS) (eds) Pöhner A, Simrock S, Thumulla J, Weber S, Wirner T (1997) Background contamination in household dust in private homes with semi- and nonvolatile organic compounds (in German). Analyse und Bewertung von Umweltschadstoffen (AnBUS) (eds)
go back to reference Robertson GL, Lebowitz MD, O’Rourke MK, Gordon S, Moschandreas D (1999) The National Human Exposure Assessment Survey (NHEXAS) study in Arizona—introduction and preliminary results. J Expo Anal Environ Epidemiol 9:427–434CrossRefPubMed Robertson GL, Lebowitz MD, O’Rourke MK, Gordon S, Moschandreas D (1999) The National Human Exposure Assessment Survey (NHEXAS) study in Arizona—introduction and preliminary results. J Expo Anal Environ Epidemiol 9:427–434CrossRefPubMed
go back to reference Savage LP, Keefe TJ, Wheeler W, Mounce F, Helwig H, Applehand F, Goes E, Goes T, Milhan G, Rench J, Taylor DK (1981) Household pesticide usage in the United States. Arch Environ Health 36:304–309PubMed Savage LP, Keefe TJ, Wheeler W, Mounce F, Helwig H, Applehand F, Goes E, Goes T, Milhan G, Rench J, Taylor DK (1981) Household pesticide usage in the United States. Arch Environ Health 36:304–309PubMed
go back to reference Schaller KH, Angerer J, Drexler H (2002) Quality assurance of biological monitoring in occupational and environmental medicine. J Chromatogr B Special Issue 778:403–417CrossRef Schaller KH, Angerer J, Drexler H (2002) Quality assurance of biological monitoring in occupational and environmental medicine. J Chromatogr B Special Issue 778:403–417CrossRef
go back to reference Walker G, Hostrup O, Hoffmann W, Butte W (1999) Biocides in household dust (in German). Gefahrstoffe- Reinhaltung der Luft 59:33–41 Walker G, Hostrup O, Hoffmann W, Butte W (1999) Biocides in household dust (in German). Gefahrstoffe- Reinhaltung der Luft 59:33–41
go back to reference Wilkes MF, Woollen BH, Marsh JR, Batten PL, Chester G (1993) Biological monitoring for pesticide exposure—the role of human volunteer studies. Int Arch Occup Environ Health 65 [Suppl] 189–192 Wilkes MF, Woollen BH, Marsh JR, Batten PL, Chester G (1993) Biological monitoring for pesticide exposure—the role of human volunteer studies. Int Arch Occup Environ Health 65 [Suppl] 189–192
go back to reference World Health Organisation (1986) Environmental health criteria 63. Organophosphorus insecticides: a general introduction. WHO, Geneva World Health Organisation (1986) Environmental health criteria 63. Organophosphorus insecticides: a general introduction. WHO, Geneva
go back to reference World Health Organisation (1990) Environmental health criteria 94. Permethrin. WHO, Geneva World Health Organisation (1990) Environmental health criteria 94. Permethrin. WHO, Geneva
go back to reference Yess NJ (1991) Residue monitoring 1991—Food and Drug Administration Pesticide Program. J AOAC Int 75:135A–157A Yess NJ (1991) Residue monitoring 1991—Food and Drug Administration Pesticide Program. J AOAC Int 75:135A–157A
Metadata
Title
Current internal exposure to pesticides in children and adolescents in Germany: urinary levels of metabolites of pyrethroid and organophosphorus insecticides
Authors
Ursel Heudorf
Jürgen Angerer
Hans Drexler
Publication date
01-01-2004
Publisher
Springer-Verlag
Published in
International Archives of Occupational and Environmental Health / Issue 1/2004
Print ISSN: 0340-0131
Electronic ISSN: 1432-1246
DOI
https://doi.org/10.1007/s00420-003-0470-5

Other articles of this Issue 1/2004

International Archives of Occupational and Environmental Health 1/2004 Go to the issue