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Exposure of Children to Creosote from Wood Impregnation on Playgrounds Dr. Andrea Boehncke, Dr. Inge Mangelsdorf Fraunhofer Institute for Toxicology and Aerosol Research – Drug Research and Clinical Inhalation, Working Group on Chemical Risk Assessment, Nikolai-Fuchs-Straße 1, D-30625 Hannover Composition of creosote A brownish-black, viscous liquid obtained by the fractional distillation of crude coal tars. Coal tars are by-products in the distillation of coal to coke or town-gas a complex mixture of high-boiling compounds (distillation range 200-400 °C) main constituents: polycylic aromatic hydrocarbons (Table 1), furthermore, phenols, creosols and xylenols There is sufficient evidence that creosote is carcinogenic to animals. This is due to the PAHs in the mixture (e.g. benzo(a)pyrene, dibenzo (a,h) anthracene). Table 1: PAHs in commercial creosotes Compound Concentration (% w/w) Acenaphthene 3.1-14.7 Anthracene 1,5-10,5 Benzo(a)pyrene 0.0004-0.35 Chrysene 0,3-3,5 Dibenz(a,h)anthracene 0.01-0.04 Fluoranthene 0,2-10,0 Fluorene 3.1-10.0 Naphthalene 1,3-18,0 Phenanthrene 1-21.0 Pyrene0.1-8.5 Total PAH content up to 85 % According to IARC (1985); ATSDR (1990); TIS (1990); Priddle & MacQuarrie (1994); Heikkilä (1987); van Rooj et al. (1993; 1998); Lehmann (1986); Sandell & Tuominen (1996) Use of creosote Widely used as an impregnation agent for wood applied outdoors such as garden fences, outdoor playing devices (e.g. sandbox edgings), – tadpoles railway sleepers etc. Mostly used in industrial applications in the so-called pressure impregnation process Significant amounts are applied in the private area creosote by brushing. From this a potential exposure of the consumer (during impregnation) and children in contact with creosote-treated playing devices (after impregnation) is to be assumed. Suitability of benzo(a)pyrene as a marker substance Benzo(a)pyrene (BaP) is a marker substance in numerous studies on PAH mixtures. This holds for the determination of BaP in the different environmental compartments and for the investigation of toxic and ecotoxic effects as well. Question: Can BaP also be used as a marker substance for this special exposure situation? Answer: Yes Reason: It was shown in a dermal carcinogenicity study with mice that two samples of creosote with differing BaP content showed the same dose- effect relationship based on BaP. Pure BaP was about 5 times less effective than as a compo- nent of creosote. This is understandable con- sidering that creosote also contains other car- cinogenic PAHs apart from BaP. The carcino- genic effect of other PAH mixtures (lubrica- ting, oil, flue gas condensation products) is of a similar order of magnitude (Mangelsdorf et al., 1998). Exposure of children to creosote from impregnated wood The possible routes of exposure are given in Figure 1. The following general assumptions were chosen. They are mainly based on the studies of Stubenrauch et al. (1995). regular stay on playgrounds in the age between 3 and 8 years, i.e. 6 years during a lifetime number of stays/year: 100 exposure time/stay: 4 hours mean body weight: 15 kg Dermal exposure Dermal exposure of children to creosote can occur 1. via freshly manually impregnated wood 2. via contaminated sand or soil 3. [via industrially impregnated wood due to exudation. Old railway sleepers may contain up to about 1600 mg/kg BaP (Rotard & Mai- lahn, 1987). It is not clear how much BaP can be released by exudation which depends strongly on weather conditions. The use of old railway sleepers on playgrounds is not recom- mended by e.g. the German Federal Institute of Consumer Protection and Veterinary Medi- cine.] 1. Via freshly manually impregnated wood Exudation is not to be expected with manually impregnated wood as the applied quantities are significantly lower and complete weathering occurs within one to two years. The estimations are based on the following assumptions: Max. BaP content of creosote: 50 ppm Skin exposure at the workplace: 1-34 ng/kg bw x d (derived from pyrene exposure at workplaces in the wood impregnating indus- try; van Rooij et al., 1993) Reduced exposure time and frequency: 4 hours/day instead of 8 hours/day 1 exposure event/year instead of ca. 200 events/years Result Possible exposure via skin contact with freshly manually impregnated wood 0.003-0.09 ng BaP/kg bw x d 2. Via contaminated sand or soil Some recent literature data on the contamina- tion of sand and soil on playgrounds in the vici- nity of sandboxes are available from Denmark. The data range from < 50 mg BaP/kg dry weight to 200 μg/kg (Miljø & Energi Ministeriet, 1996). The estimations are based on the following assumptions: Average BaP content of sand/soil: 60 μg/kg Exposed body surface: 440 cm 2 (inner parts of hands) Adhesion factor for sand/soil: 0.5-1.7 mg/cm 2 (Stubenrauch et al., 1995; AGLMB, 1995) Result Possible exposure via skin contact with contaminated sand or soil: 0.2-0.8 ng BaP/kg bw x d FRG: 45-3490 ppm; 70%ile 500 ppm NL: < 4-20 ppm SU: 300-1200 ppm PO: 300 ppm GUS:2000 ppm Oral exposure Indirect oral exposure due to clearance of in- haled particles is assumed to be negligible: inhalation exposure can be shown to be very low (see below) BaP adsorbs especially to small particles which have a high retention time in the lung. However, small children in particular tend to have a significant uptake of sand or soil during their playing activities. This route of exposure is quantified with the following assumptions as a basis: Uptake of contaminated sand or soil: 0.5-1 g/exposure event (dependent on age; Stubenrauch et al., 1994a) Average BaP content of sand/soil: 60 μg/kg (see above) Result Possible oral exposure to contaminated sand or soil: 0.5-1 ng BaP/kg bw x d Inhalation exposure Inhalation exposure of BaP from creosote is only possible by inhalation of contaminated dust. The following assumptions were compiled from the literature: Inhalation rate of children: 0.13-1.8 m 3 /h (Stu- benrauch et al., 1994a) Dust content of air on playing fields: 6.6 mg/m 3 (Stubenrauch et al, 1994a) Dust retention in the lung: 40% (WHO, 1987) BaP content of dust: 60 μg/kg (see above) Result Possible inhalation exposure to contaminated dust: 0.001-0.02 ng BaP/kg bw x d Conclusion Most relevant exposure paths: dermal exposure to contaminated sand or soil oral exposure to contaminated sand or soil. But estimations are highly uncertain due to numerous assumptions the Scientific Committee of Toxicity, Ecotoxi- city and the Environment (CSTEE) estimated a lifetime risk of ca. 10-4 for a BaP dose of 1 ng/kg bw x d (CSTEE, 1999) this would give clear reason for concern especially in the context of cumulative expo- sure (e.g. exposure via food, ambient air). Probabilistic methods would be a helpful tool to refine the exposure assessment. Children playing outdoors Creosote impregnated wood Direct contact Skin Volatilization Air Leaching Soil, sand Ingestion Permeation Ingestion Permeation Inhalation Ingestion References AGLMB (1995) Standards zur Expositionsabschätzung. Arbeitsgemeinschaft der leitenden Medizinalbeamtin- nen und -beamten der Länder, Bericht des Ausschusses für Umwelthygiene. Hrg. Behörde für Arbeit, Gesund- heit und Soziales, Hamburg ATSDR (1990) Toxicological profile for polycyclic aroma- tic hydrocarbons., U.S. Department of Health & Human Services Agency for Toxic Substances and Disease Registry CSTEE (1999) Opinion (revised) on cancer risk to consu- mers from creosote containing less than 50 ppm benzo- [a]-pyrene and/or from wood treated with such creosote and estimation of respective magnitude expressed at the 8th CSTEE meeting, Brussels, 4th of March Mangelsdorf I, Boehncke A & Holländer W (1998) Aus- wertung einer dermalen Kanzerogenitätsstudie mit zwei verschiedenen Teerölprodukten. Fraunhofer Institut für Toxikologie und Aerosolforschung, Hannover. Im Auf- trag des Bundesministeriums für Umwelt, Naturschutz und Reaktorsicherheit, Bonn Heikkilä PR, Hämeilä M, Pyy L, Raunu P (1987) Exposure to creosote in the impregnation and handling of impregnated wood. Scand. J. Work Eniron. Health 13: 431-437 IARC (1985) Polycyclic aromatic compounds, Part 4, bitumens, coal-tars and derived products, shale-oils and soots. In: IARC (ed.) IARC monographs on the Evaluation of the Carcinogenic Risk of Chemicals to Humans. Lyon/France Lehmann E, Auffarth J, Häger J, Rentel KH & Altenburg H (1986) Massenverhältnisse ausgewählter PAH in Pro- dukten auf Steinkohlenteer-Basis. Staub-Reinhalt Luft 46: 128-131 Priddle & MacQuarrie (1994) Dissolution of creosote in groundwater: an experimental and modeling investiga- tion. J Contam Hydrol 15: 27-56 Rotard W & Mailahn W (1987) Gas chromatographic- mass spectrometric analysis of creosotes extracted from wooden sleepers installed in playgrounds. Anal Chem 59: 65-69 Sandell E & Tuominen J (1996) The impact of the use and disposal of creosote impregnated railway ties on a freshwater supply area in southern Finland. Polycyclic Aromat Compd 11: 83-90 Stubenrauch S, Hempfling R, Simmleit N, Mathews T & Doetsch P (1994) Abschätzung der Schadstoffexposi- tion in Abhänigkeit von Expositionsszenarien und Nut- zergruppen. II. Vorschläge für orale Aufnahmeraten von Boden, Badeseewasser und Nahrungsmitteln des Eigen- anbaus. Umweltwiss Schadst -Forsch 6: 165-174 Stubenrauch S, Hempfling R, Simmleit N & Doetsch P (1994) Abschätzung der Schadstoffexposition in Abhän- gigkeit von Expositionsszenarien und Nutzergruppen. III. Vorschläge für inhalative Aufnahmeraten. Umweltwiss Schadst -Forsch 6: 289-296 Stubenrauch S, Hempfling R & Simmleit N (1995) Abschätzung der Schadstoffexposition in Abhänigkeit von Expositionsszenarien und Nutzergruppen. IV. Vor- schläge für die Ableitung dermaler Aufnahmeraten. Umweltwiss Schadst -Forsch 7: 37-461995 Van Rooij JGM, Van Lieshout EMA, Bodelier-Bade MM & Jongeneelen FJ (1993) Effect of the reduction of skin contamination on the internal dose of creosote workers exposed to polycyclic aromatic hydrocarbons. Scand J Work Environ Health 19: 200-207 Van Roij (1998) Personal communication WHO (1987) Polynuclear aromatic hydrocarbons (PAH). In: Air quality guidelines for Europe, WHO Reg. Pub., Eur. Series No. 23, Chapter 11. 105-117 Fig. 1: Possible routes of exposure of children to creosote Exposure scenario Source Release mechanism Target Route of exposure

Exposure of Children to Creosote From Wood Impregnation on Playgrounds

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Exposure of Children to Creosote from Wood Impregnation on PlaygroundsDr. Andrea Boehncke, Dr. Inge Mangelsdorf Fraunhofer Institute for Toxicology and Aerosol Research – Drug Research and Clinical Inhalation, Working Group on Chemical Risk Assessment, Nikolai-Fuchs-Straße 1, D-30625 Hannover

Composition of creosote

– A brownish-black, viscous liquid– obtained by the fractional distillation of crude

coal tars. Coal tars are by-products in thedistillation of coal to coke or town-gas

– a complex mixture of high-boiling compounds(distillation range 200-400 °C)

– main constituents:polycylic aromatic hydrocarbons (Table 1), furthermore, phenols, creosols and xylenols

There is sufficient evidence that creosote iscarcinogenic to animals. This is due to the PAHsin the mixture (e.g. benzo(a)pyrene, dibenzo(a,h) anthracene).

Table 1: PAHs in commercial creosotes

Compound Concentration (% w/w)

Acenaphthene 3.1-14.7Anthracene 1,5-10,5Benzo(a)pyrene 0.0004-0.35Chrysene 0,3-3,5Dibenz(a,h)anthracene 0.01-0.04Fluoranthene 0,2-10,0Fluorene 3.1-10.0Naphthalene 1,3-18,0Phenanthrene 1-21.0Pyrene0.1-8.5Total PAH content up to 85 %

According to IARC (1985); ATSDR (1990); TIS (1990); Priddle & MacQuarrie (1994); Heikkilä (1987); van Rooj et al. (1993; 1998); Lehmann (1986); Sandell & Tuominen (1996)

Use of creosote

– Widely used as an impregnation agent forwood applied outdoors such as – garden fences, outdoor playing devices (e.g.

sandbox edgings), – tadpoles– railway sleepers etc.

– Mostly used in industrial applications in theso-called pressure impregnation process

– Significant amounts are applied in the privatearea creosote by brushing.

From this a potential exposure of the consumer(during impregnation) and children in contactwith creosote-treated playing devices (afterimpregnation) is to be assumed.

Suitability of benzo(a)pyrene as amarker substance

– Benzo(a)pyrene (BaP) is a marker substance innumerous studies on PAH mixtures. This holdsfor the determination of BaP in the differentenvironmental compartments and for theinvestigation of toxic and ecotoxic effects aswell.

– Question: Can BaP also be used as a marker substancefor this special exposure situation?

– Answer: Yes

– Reason: It was shown in a dermal carcinogenicity studywith mice that two samples of creosote withdiffering BaP content showed the same dose-effect relationship based on BaP. Pure BaP wasabout 5 times less effective than as a compo-nent of creosote. This is understandable con-sidering that creosote also contains other car-cinogenic PAHs apart from BaP. The carcino-genic effect of other PAH mixtures (lubrica-ting, oil, flue gas condensation products) is of a similar order of magnitude (Mangelsdorfet al., 1998).

Exposure of children to creosotefrom impregnated wood

The possible routes of exposure are given inFigure 1. The following general assumptionswere chosen. They are mainly based on the studies of Stubenrauch et al. (1995).

– regular stay on playgrounds in the age between 3 and 8 years, i.e. 6 years during alifetime

– number of stays/year: 100– exposure time/stay: 4 hours– mean body weight: 15 kg

Dermal exposure

Dermal exposure of children to creosote canoccur 1.via freshly manually impregnated wood2.via contaminated sand or soil 3.[via industrially impregnated wood due to

exudation. Old railway sleepers may containup to about 1600 mg/kg BaP (Rotard & Mai-lahn, 1987). It is not clear how much BaP can be released by exudation which dependsstrongly on weather conditions. The use of oldrailway sleepers on playgrounds is not recom-mended by e.g. the German Federal Instituteof Consumer Protection and Veterinary Medi-cine.]

1. Via freshly manually impregnated woodExudation is not to be expected with manuallyimpregnated wood as the applied quantities aresignificantly lower and complete weatheringoccurs within one to two years. The estimationsare based on the following assumptions:

– Max. BaP content of creosote: 50 ppm– Skin exposure at the workplace: 1-34 ng/kg

bw x d (derived from pyrene exposure at workplaces in the wood impregnating indus-try; van Rooij et al., 1993)

– Reduced exposure time and frequency:4 hours/day instead of 8 hours/day1 exposure event/year instead of ca. 200events/years

Result

Possible exposure via skin contact with freshlymanually impregnated wood0.003-0.09 ng BaP/kg bw x d

2. Via contaminated sand or soilSome recent literature data on the contamina-tion of sand and soil on playgrounds in the vici-nity of sandboxes are available from Denmark.The data range from < 50 mg BaP/kg dry weightto 200 µg/kg (Miljø & Energi Ministeriet, 1996).The estimations are based on the followingassumptions:

– Average BaP content of sand/soil: 60 µg/kg – Exposed body surface: 440 cm2 (inner parts of

hands)– Adhesion factor for sand/soil: 0.5-1.7 mg/cm2

(Stubenrauch et al., 1995; AGLMB, 1995)

Result

Possible exposure via skin contact with contaminated sand or soil:0.2-0.8 ng BaP/kg bw x d

FRG: 45-3490 ppm; 70%ile ≤500 ppm

NL: < 4-20 ppmSU: 300-1200 ppmPO: 300 ppmGUS:2000 ppm

Oral exposure

Indirect oral exposure due to clearance of in-haled particles is assumed to be negligible: – inhalation exposure can be shown to be very

low (see below)– BaP adsorbs especially to small particles which

have a high retention time in the lung.

However, small children in particular tend tohave a significant uptake of sand or soil duringtheir playing activities. This route of exposure isquantified with the following assumptions as abasis:

– Uptake of contaminated sand or soil: 0.5-1 g/exposure event (dependent on age; Stubenrauch et al.,1994a)

– Average BaP content of sand/soil: 60 µg/kg(see above)

Result

Possible oral exposure to contaminated sand or soil:0.5-1 ng BaP/kg bw x d

Inhalation exposure

Inhalation exposure of BaP from creosote is onlypossible by inhalation of contaminated dust.The following assumptions were compiled fromthe literature:

– Inhalation rate of children: 0.13-1.8 m3/h (Stu-benrauch et al., 1994a)

– Dust content of air on playing fields: 6.6 mg/m3 (Stubenrauch et al, 1994a)

– Dust retention in the lung: 40% (WHO, 1987)– BaP content of dust: 60 µg/kg (see above)

Result

Possible inhalation exposure to contaminateddust:0.001-0.02 ng BaP/kg bw x d

Conclusion

Most relevant exposure paths:– dermal exposure to contaminated sand or soil– oral exposure to contaminated sand or soil.

But– estimations are highly uncertain due to

numerous assumptions– the Scientific Committee of Toxicity, Ecotoxi-

city and the Environment (CSTEE) estimated a lifetime risk of ca. 10-4 for a BaP dose of 1 ng/kg bw x d (CSTEE, 1999)

– this would give clear reason for concern– especially in the context of cumulative expo-

sure (e.g. exposure via food, ambient air).

Probabilistic methods would be a helpful tool torefine the exposure assessment.

Children playing outdoors

Creosote impregnated wood

Direct contact

Skin

Volatilization

Air

Leaching

Soil, sand

Ingestion Permeation Ingestion PermeationInhalation Ingestion

References

AGLMB (1995) Standards zur Expositionsabschätzung.Arbeitsgemeinschaft der leitenden Medizinalbeamtin-nen und -beamten der Länder, Bericht des Ausschussesfür Umwelthygiene. Hrg. Behörde für Arbeit, Gesund-heit und Soziales, Hamburg

ATSDR (1990) Toxicological profile for polycyclic aroma-tic hydrocarbons., U.S. Department of Health & HumanServices Agency for Toxic Substances and Disease Registry

CSTEE (1999) Opinion (revised) on cancer risk to consu-mers from creosote containing less than 50 ppm benzo-[a]-pyrene and/or from wood treated with such creosoteand estimation of respective magnitude expressed atthe 8th CSTEE meeting, Brussels, 4th of March

Mangelsdorf I, Boehncke A & Holländer W (1998) Aus-wertung einer dermalen Kanzerogenitätsstudie mit zweiverschiedenen Teerölprodukten. Fraunhofer Institut fürToxikologie und Aerosolforschung, Hannover. Im Auf-trag des Bundesministeriums für Umwelt, Naturschutzund Reaktorsicherheit, Bonn

Heikkilä PR, Hämeilä M, Pyy L, Raunu P (1987) Exposureto creosote in the impregnation and handling ofimpregnated wood. Scand. J. Work Eniron. Health 13: 431-437

IARC (1985) Polycyclic aromatic compounds, Part 4, bitumens, coal-tars and derived products, shale-oils andsoots. In: IARC (ed.) IARC monographs on the Evaluationof the Carcinogenic Risk of Chemicals to Humans.Lyon/France

Lehmann E, Auffarth J, Häger J, Rentel KH & AltenburgH (1986) Massenverhältnisse ausgewählter PAH in Pro-dukten auf Steinkohlenteer-Basis. Staub-Reinhalt Luft46: 128-131

Priddle & MacQuarrie (1994) Dissolution of creosote ingroundwater: an experimental and modeling investiga-tion. J Contam Hydrol 15: 27-56

Rotard W & Mailahn W (1987) Gas chromatographic-mass spectrometric analysis of creosotes extracted fromwooden sleepers installed in playgrounds. Anal Chem59: 65-69

Sandell E & Tuominen J (1996) The impact of the useand disposal of creosote impregnated railway ties on afreshwater supply area in southern Finland. PolycyclicAromat Compd 11: 83-90

Stubenrauch S, Hempfling R, Simmleit N, Mathews T & Doetsch P (1994) Abschätzung der Schadstoffexposi-tion in Abhänigkeit von Expositionsszenarien und Nut-zergruppen. II. Vorschläge für orale Aufnahmeraten vonBoden, Badeseewasser und Nahrungsmitteln des Eigen-anbaus. Umweltwiss Schadst -Forsch 6: 165-174

Stubenrauch S, Hempfling R, Simmleit N & Doetsch P(1994) Abschätzung der Schadstoffexposition in Abhän-gigkeit von Expositionsszenarien und Nutzergruppen. III.Vorschläge für inhalative Aufnahmeraten. UmweltwissSchadst -Forsch 6: 289-296

Stubenrauch S, Hempfling R & Simmleit N (1995)Abschätzung der Schadstoffexposition in Abhänigkeitvon Expositionsszenarien und Nutzergruppen. IV. Vor-schläge für die Ableitung dermaler Aufnahmeraten.Umweltwiss Schadst -Forsch 7: 37-461995

Van Rooij JGM, Van Lieshout EMA, Bodelier-Bade MM &Jongeneelen FJ (1993) Effect of the reduction of skincontamination on the internal dose of creosote workersexposed to polycyclic aromatic hydrocarbons. Scand JWork Environ Health 19: 200-207

Van Roij (1998) Personal communication

WHO (1987) Polynuclear aromatic hydrocarbons (PAH).In: Air quality guidelines for Europe, WHO Reg. Pub.,Eur. Series No. 23, Chapter 11. 105-117

Fig. 1: Possible routes of exposure of children to creosote

Exposure scenario

Source

Release mechanism

Target

Route of exposure