Revised reference value for pentachlorophenol in morning urine

Revised reference value for pentachlorophenol in morning urine

ARTICLE IN PRESS Int. J. Hyg. Environ. Health 210 (2007) 741–744 www.elsevier.de/ijheh Revised reference value for pentachlorophenol in morning urin...

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ARTICLE IN PRESS

Int. J. Hyg. Environ. Health 210 (2007) 741–744 www.elsevier.de/ijheh

Revised reference value for pentachlorophenol in morning urine C. Schulza,, W. Butteb a

Federal Environment Agency, Berlin, Germany Carl von Ossietzky University Oldenburg, Institute for Pure and Applied Chemistry, Oldenburg, Germany

b

Received 1 June 2006; received in revised form 27 October 2006; accepted 2 November 2006

Abstract Reference values are continuously derived by the Human Biomonitoring Commission of the German Federal Environment Agency to give help in assessing the exposure of individuals or population groups in comparison to the background exposure. As environmental conditions may change reference values should be checked periodically and they have to be updated, if new data become available. The results of the German Environmental Survey 1998 (GerES III) showed the decreasing pentachlorophenol (PCP) exposure of the German adult population. Therefore, the reference value for PCP in morning urine was lowered: from 8 to 5 mg/l for adults (aged 18–69 years) living in homes where wood preservatives had not been used. r 2006 Elsevier GmbH. All rights reserved. Keywords: Human biomonitoring; Reference values; Urine; Pentachlorophenol; Environmental medicine; Germany

Introduction Pentachlorophenol (PCP) is one of the most important environmental chemicals due to its toxicity, its contamination with dioxins and its ubiquitous distribution in the environment. Reference values for the German population were deduced for the first time in 1997 by the German Human Biomonitoring Commission (1997). The first updating of reference values was carried out in 1999 (Human Biomonitoring Commission, 1999). The German Environmental Survey 1998 (GerES III), a population-representative study (Becker et al., 2002a, 2003; Krause et al., 1998), is the basis for a renewed updating of reference values for PCP in morning urine of adults (Human Biomonitoring Com-

Corresponding author. Tel.: +49 30 89035465; fax: +49 30 89031830. E-mail address: [email protected] (C. Schulz).

1438-4639/$ - see front matter r 2006 Elsevier GmbH. All rights reserved. doi:10.1016/j.ijheh.2006.11.004

mission, 2004). This updating represents the decreasing PCP exposure of the German population. In Germany, the Human Biomonitoring Commission of the German Federal Environment Agency was established in 1992 to clarify fundamental and practical issues related to human biomonitoring (HBM) (http:// www.umweltbundesamt.de/uba-info-daten-e/daten-e/ monitor/index.htm, date: October 20, 2006). According to the commission, HBM is an important tool in environmental medicine to assess and evaluate the internal exposure levels of the general population, population subgroups, and individuals to environmental pollutants. The working principles and the working procedures of the commission have been summarized by Ewers et al. (1999) and Schulz et al. (2007). Reference values must be revised periodically according to changes in the exposure of the general population to environmental pollutants. New and revised reference values were reported for persistent organic pollutants (Wilhelm et al., 2003), for trace elements (Wilhelm et al., 2004),

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for metabolites of pyrethroid and organophosphorous insecticides (Heudorf et al., 2006) and for arsenic, cadmium, lead and mercury in blood or urine of children (Wilhelm and Schulz, 2006).

General remarks The reference value is defined as the 95th percentile of the distribution of concentrations of a specific compound or element in the relevant body fluid of a reference population (Ewers et al., 1999; Schulz et al., 2007). It is deduced from the 95% confidence interval of the 95th percentile and should be a rounded value, if possible. Basis for this procedure is a guideline of the International Union of Pure and Applied Chemistry (IUPAC) (1997). Reference values for pollutants in urine are expressed as mg/l urine (and no longer as mg/g creatinine). In line with the WHO’s recommendations (1996), the commission decided when deriving reference values to include only urine samples with creatinine levels in the range between 0.3 and 3.0 g/l. For HBM in environmental medicine, it is recommended that in individual cases of values exceeding the reference value a repeated sampling should be performed and care should be taken that the urine exhibits a normal dilution, i.e., a creatinine content between 0.5 and 2.5 g/l (Human Biomonitoring Commission, 2005). It has to be emphasized that reference values are statistically derived values to give criteria to estimate the exposure of individuals or groups of persons as ‘‘elevated’’ or ‘‘not elevated’’. Thus, they cannot be used for a health-related evaluation of HBM data. Nevertheless, the reference values permit to assess the exposure of individuals or population groups compared to the ubiquitous background exposure. For assessing the exposure from the viewpoint of environmental medicine or toxicology HBM values have to be applied (Human Biomonitoring Commission, 1996).

Data basis The GerES III is, like its two precursors, a population-representative study characterizing a cross-section of the population living in Germany (Krause et al., 1998; Seifert et al., 2000). Samples were taken between October 1997 and March 1999. The objectives of GerES are, inter alia, to evaluate the body burden of pollutants of the general population, to investigate the contribution of different compartments (dust, air, water, food) to the body burden and to develop models to assess exposure. Altogether 4822 adults at the age of 18–69 years participated in this survey. PCP concentrations in morning urine were analyzed for 691 persons (342

women and 349 men) using GC–MS (Angerer, 2001). Additionally PCP concentrations were measured in 714 house dust samples (o2 mm fraction) using GC–ECD (Butte et al., 2001; Walker et al., 1999). Methods applied in GerES III (random sampling, analytical methods, statistical data treatment, etc.) as well as a description of the data obtained for HBM were published by Becker et al. (2002a). Results for PCP in morning urine are described here in detail.

Results and discussion PCP concentrations in morning urine covered the range between o0.6 mg/l (limit of quantification) and 19.1 mg/l (o0.3–16.8 mg/g creatinine), with a geometric mean of 1.04 mg/l (0.83 mg/g creatinine) and a 95th percentile of 13 mg/l (11 mg/g creatinine) (Becker et al., 2003). The HMB I value for PCP of 25 mg/l and of 20 mg/ g creatinine (Human Biomonitoring Commission, 1997) were not exceeded in any of the urine samples. Results of GerES III demonstrated that PCP concentrations in urine of adults are significantly lower in 1998 compared to 1990/92 (Becker et al., 2002a). This decline in exposure to PCP after enforcing the ‘‘Pentachlorphenol-Verbotsverordnung’’ (1989) (regulation to ban PCP) was also observed in other studies (Federal Environment Agency, 1999). For subjects declaring that wood preservatives (WP) in their households had been used higher concentrations of PCP in urine were found (Obi-Osius et al., 2005). But differences are small for the medians: 1.3 mg/l (use of WP) compared to 1.0 mg/l (no use of WP); differences are more distinct for the 95th percentile: 6.9 mg/l (use of WP) compared to 4.9 mg/l (no use of WP) (Becker et al., 2002a, Table 1). For a part of the population participating in GerES III (n ¼ 741) PCP in house dust (o2 mm fraction) was analyzed. About 70% of the samples showed PCP concentrations exceeding the limit of quantification of 0.1 mg/kg. The median was 0.2 mg/ kg, the 95th percentile was 2.9 mg/kg and the maximum value was 32.2 mg/kg (Becker et al., 2002b). For 546 subjects, PCP concentrations in morning urine as well as in house dust were determined. For this collective a weak but significant correlation was observed. Spearman’s rank correlation coefficient was rs ¼ 0.12 (po0.01) for the correlation of PCP in house dust versus concentrations of PCP in morning urine. For several decades, ending in 1978, PCP was the fungicide most frequently used for wood preservation in Germany (Human Biomonitoring Commission, 1997). The widespread application of WP containing PCP and its uncontrolled use by non-professionals is of principal importance regarding environmental health problems. This is due to the persistence of PCP in the indoor environment and the fact that even some decades after

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Table 1. Pentachlorophenol in morning urine (mg/l) of adults depending on the application of wood preservatives in the home (Becker et al., 2002a) and reference value (Human Biomonitoring Commission, 2004) Group

n

noLOQ

P50

All 691 175 1.0 Application of wood preservatives in the home* Yes 74 15 1.3 No 585 156 1.0

P95

GM

5.0

1.04

6.9 4.9

1.30 1.00

CI 95 PP

Reference value

3.95–4.98

5.0

n ¼ number of samples; LOQ ¼ limit of quantification; noLOQ ¼ number of values below LOQ, values below LOQ are set at LOQ/2 for calculation purposes; P50 ¼ 50th percentile (median); P95 ¼ 95th percentile; GM ¼ geometric mean; CI 95 PP ¼ approximate 95%-confidence interval for the 95th population percentile. *Significant difference for the GM (po0.05, t-test).

an application of PCP concentrations are distinctly higher in treated compared to untreated wood. As PCP is continuously emitted from the treated wood elevated concentrations in house dust and in indoor air are expected (Human Biomonitoring Commission, 1997). Thus, results obtained with GerES III seem plausible, i.e., slightly higher concentrations of PCP in morning urine for persons living in households where WP were used or that had higher concentrations of PCP in house dust.

Further perspectives

Reference value for PCP in morning urine

This report is based on a consensus paper of the Human Biomonitoring Commission. The authors thank the other members of the Commission (J. Angerer, R. Eckard, U. Ewers, B. Heinzow, U. Heudorf, A. Kappos, H. Kruse, M. Schwenk and M. Wilhelm) for their cooperation.

On the basis of data obtained with GerES III the Human Biomonitoring Commission (2004) revised the reference value for PCP in morning urine: 5 mg PCP/l morning urine (adults, aged 18–69 years, living in homes where no WP had been used). Urine samples with creatinine concentrations o0,3–43 g/l are excluded.

As soon as data from the German Environmental Survey for Children 2003/2006 (GerES IV) are available (http://www.umweltbundesamt.de/survey-e/us03/uprog. htm), the Human Biomonitoring Commission will provide reference values for PCP in urine of children.

Acknowledgements

References Recommendations in cases of values exceeding the reference value If the PCP concentration in urine exceeds the reference value, the measurement should be repeated for control and care should be taken in repeating the measurement that the creatinine concentration is within the range of 0.5–2.5 g/l urine. If case concentrations of PCP in morning urine reliably exceed the reference value, one should not only consider WP as a source, but one should also take into account leather from clothes and upholstery impregnated with PCP as well as a longer staying abroad (Heudorf, 2002; Heudorf et al., 2003). If reliable (checked several times) measurements show a value above the reference value, they should induce an environmental medicine-based search for sources. Such search should be carried out in a proportionate way. It must be emphasized that reference values are statistically derived and do not represent toxicologically derived biological exposure limits.

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