United States Environmental Protection Agency Atmospheric Research and Exposure Assessment Laboratory Research Triangle Park, NC 27711 Research and Development EPA/600/S3-90/030 June 1990 SEPA Project Summary Field Evaluation of a High Volume Surface Sampler for Pesticides in Floor Dust W. T. Budd, J. W. Roberts, and M. G. Ruby House dust and the pollutants carried with it are potentially important contributors to total exposure through the pathways of inhalation, ingestion and skin pen- etration, especially for small children. Pesticides may be one of the more important contaminants of house dust. The full report describes a pilot study conducted as a part of the Non- Occupational Pesticide Exposure Study (NOPES), which provides pre- liminary information on the pesticide content of floor dust. A high volume surface sampler (HVS2) for the collection of house dust and the semivolatile organics in house dust has been developed and tested in the laboratory. This study also served as a field test and initial validation study of the HVS2. The HVS2 is designed to collect more than 2 g of floor dust from a rug in an average clean residence in a few minutes. Such a large sample could be used in bioassays or analyzed for a variety of contaminants. This study was conducted in nine houses in the Jacksonville, Florida Phase III segment of the NOPES study. Both the NOPES questionnaire and a supplemental questionnaire were administered in each household to develop information on pesticide usage and other variables that might be related to the floor dust samples. All samples were collected from carpeted surfaces. The samples were collected and processed using previously pub- lished procedures. Both the HVS2 and the procedures were found to be generally satisfactory. An average of 3.2 m2 (34 ft2) was necessary to collect a 2 g sample. The total time for collecting a single sample, including sample processing, clean- up of the HVS2, and travel time, was approximately 4 hours. The samples were analyzed for 33 pesticides by GC/ECD andGC/MS following the NOPES standard procedures. High concentrations of interfering compounds in some samples required substantial dilution before they could be analyzed. As a result, other analytes were diluted below their detection limit. On average, 7.5 target pesticides were observed in the indoor air samples and 11.8 in the floor dust. The number observed in the floor dust ranged from 2 to 23. Thirteen of the pesticides were observed only in the floor dust. The most consistently observed pesticides were chlOrpy- rifos, with a median concentration of about 5 ppm in the dust, and chlordane, with a median concentra- tion of approximately 6 ppm. The ------- median surface loading of chtorpyrifos was approximately 6 yg/m2 and of chlordane, about 13 ug/m2. No significant correlation between surface loading and dust concentration was seen for these or most other pesticides. Several pesticides were observed in floor dust which have not been in widespread use for many years. Exploratory statistical analyses suggest that a relationship may exist between the measured concentra- tions of pesticides in the dust and in the air for some pesticides. A relationship was observed between the number of pesticides detected and the age of the house. The HVS2's PUF plug adsorber was necessary for the accurate measurement of five pesticides. The source of the pesticides on the PUF plug (room air or blow off from the glass fiber filter) was not determined nor Is it clear why these five pesticides are more likely to be found in the PUF plug. A supplemental experiment indicates a relationship between blowoff and vapor pressure. This Project Summary was developed by EPA's Atmospheric Research and Exposure Assessment Laboratory, Research Triangle Park, NC, to announce key findings of the research project that is full-y documented In a separate report of the same title (see Project Report ordering Information at back). Introduction The Non-Occupational Pesticide Exposure Study (NOPES) was designed to gather information on total human exposure to selected pesticides among persons not occupationally exposed, using the Total Exposure Assessment Methodology. During Phase I and Phase II of NOPES, measurements were taken to permit estimates of human exposure through air, drinking water, and dermal contact. The full report describes a pilot study during the NOPES Phase III activities which provides preliminary information on possible human exposure to pesticides through the additional medium of household dust. The importance of routes of exposure other than inhalation has been increasingly recognized in recent studies. The Health and Safety Plans for the Hyde Park disposal site in Niagara Falls, New York developed under a Superfund consent decree require the monitoring of homes for contamination of the house dust. However, i prior to this study, no validated procedure existed to make such measurements. I The ingestion of pollutants deposited on soil and dust (particularly house dust) is expected to b|e especially important for very young children, because of their lower body weight and frequent hand-to- mouth activity.! The toddler has only about one-fifth [the body weight of an adult and ingests an estimated 2.5 times as much dust> which increases the potential health frisk to the child by at least 12 times. ^Further, the risk to such children will be' increased by the early stage of development of their organs, nervous system, and immune system. Estimates of '• the risks posed by pesticides and other semivolatile chemicals should therefore include an evaluation of the dust-mediated pathway. Validation of'a method for sampling surface dust ife necessary if reliable measurements • are to be made. The study reported here also served as a field test and initial validation study of a new surface dust sahpling methodology, the High Volume Surface Sampler (HVS2), constructed by [Cascade Stack Sampling Systems (CS3). The HVS2 was designed and developed (Roberts and Ruby, 1988) under EPA spbnsorship as a way to collect rembvablesurface dust accumulations on indoor surfaces (e.g., rugs and floors); and outdoor fugitive dust surfaces (e.gj., bare ground at a contaminated earth site). The HVS2 has been extensively tested in the laboratory. It is designed to collect several grams of dust in a few minutes from a rug or bare floor in an average house. Such a large sample could be used in bioassays or analyzed for a variety of contaminants by separate techniques. Because many of the environmental pollutants of most concern in the dust matrix are semivolatile organics, the HVS2 has been, and is here, carefully studied for its ability to capture these organic compounds. This study involved nine houses in the Phase III Jacksonville NOPES set. The HVS2 was useci to collect a sample of dust in each house. Analysis included the dust loading on the surface and the concentration o'f pesticides in the dust. The primary purposes of this study were to field test th<3 HVS2 to validate the methodology, to obtain preliminary data on the amount and characteristics of dust in residences, and to obtain preliminary data on the species and concentration of pesticides in house dust. The full repoijt provides information on the practical aspects of field operations with the HVS2, the ability of the HVS2 to retain the collected pesticide material, the variation in dust loading observed in the nine houses, the loading and concentrations of pesticides in house dust in the nine houses, and a comparison of the concentrations in the air and in the dust. Data Collection Methods The sampling activities for this study were integrated with the NOPES Phase III sampling activities. The houses for floor dust sampling were obtained opportunistically from volunteers during one week of routine sampling activity. The standard NOPES samples were collected in each household, including indoor and outdoor air, in addition to the floor dust sample. The selection of the floor area within the house to be sampled was determined primarily by convenience for sampling and the probability that a sufficiently large dust sample could be collected in a short period of time. No attempt was made to presurvey the entire house in order to select a representative area or an area where children would be likely to play. All the samples in this study are from carpeted surfaces'. The NOPES Study Questionnaire was administered in a personal interview. The Study Questionnaire requested demographic data for the individual respondent, any occupational exposure to pesticides, the potential for pesticide use in the home, and an inventory of all pesticides currently in the house. In the floor dust sample houses an additional questionnaire was administered. This questionnaire included queries on the type and frequency of floor cleaning, the number of cigarettes smoked in the household, and the frequency of fireplace or woodstove use, if one were present. Floor dust sampling was carried out using the HVS2 and the sampling procedures described by Roberts and Ruby (1988). In brief, the HVS2 is a high- powered vacuum cleaner equipped with a nozzle that can be adjusted to a specific static pressure within the nozzle, a cyclone to separate the larger particles from the air stream immediately after their removal from the surface, a high efficiency quartz fiber filter for particles, and (optionally) a polyurethane foam (PUF) plug adsorber for semivolatile organic compounds. The HVS2 has been shown to collect a consistent amount of the material on either a plush or level loop carpet, the two most commonly found residential carpets. With a standard test dust it will ------- collect approximately 30% of the material in the test dust, which was less than 150 jim. The recommended test procedures for the HVS2 (Roberts and Ruby, 1988) include calibration of the required measuring instruments, pretest preparation of the HVS2 and supplies, the procedures for sampling, and a procedure for clean up in the field between samples. The sampling procedure calls for laying out eight 46 by 137 cm (18 by 54 in.) rectangles, setting the HVS2 flowrate and nozzle pressure drop, sampling four of these rectangles, and then continuing the sampling of the additional rectangles until 2 g of material has been collected. Field Operations In addition to obtaining preliminary data on the amount and characteristics of dust in homes and preliminary data on the species and concentration of pesticides in house dust, this field study provided an opportunity to validate the High Volume Surface Sampler and to field test the sampling methodology. The latter included an evaluation of the practicality of the sampling, cleanup, and analysis procedures, the approximate times required to perform each of the tasks, a determination of the amount of sample that could be realistically collected in a normal range of houses, and an evaluation of the acceptability of the HVS2 by the residents of the sampled house. Although the HVS2 weighs about 25 kg (55 pounds), it could be carried into the house by one person. After it was carried into the house, the floors were examined to locate areas where the 46 by 137 cm (18 by 54 in.) sample sections could be laid out. A folding frame was used as a template for marking the selected sampling areas with masking tape. It was necessary to use from 1 to 13 (average of 5) sampling areas to collect the required 2 g of sample. The sample areas contain 0.63 m2 (6.8 ft2). Because the amount of dust on the floor varied widely, it was difficult to estimate prior to sampling how many sample areas would be required. The sampling continued over additional sample sections until about 2 g of material were collected. On average, this required less than 7 minutes. The HVS2 was cleaned between runs using brushes and a mixed solvent (50% acetone/50% hexane) rinse on the entire sampling train between the nozzle and the PDF plug holder. The cyclone catch was weighed and then seived to less than 150 pm, using a shaker and sieves following ASTM standard method 422-63. Results Seven of the nine sample sites were single-family detached houses and the remaining two were mobile homes. In all but one house, most of the floors (other than kitchen and bathroom) were carpeted. Dust Loading The floor dust loadings at each site were determined by dividing the total sample collected in the cyclone and the fraction of that less than 150 pm by the total area sampled. The results are presented in Table 1. The two houses which have the greatest loading are also the two houses which were not using a vacuum. The ratio of the fine fraction to the total dust load is about 0.5, if the two high loading houses are not included. Table 1. Total and Fine Fraction Dust Loading by Household Household 1 227-21 6 0753-039 1064-014 0490-026A 0490-026B 1440-01 6A 1 440-0 16B 1647-001 1064-011 0966-021 0782-038 Total Dust load (g/m2) 10.8 4.2 0.3 2.2 0.8 1.4 4.3 0.8 6.6 33.7 812.7 Dust <150 Itm load (g/m2) 6.6 3.0 0.1 1.2 0.3 1.0 1.1 0.3 4.7 23.3 168.9 Pesticide Loadings and Concentrations in Air and Dust The loading of the NOPES target pesticides was calculated by dividing the total mass of the pesticide by the area sampled. The concentration of the pesticide in the collected dust was calculated by dividing the total mass of pesticide by the mass of the fine fraction of the cyclone catch plus the mass on the quartz fiber filter. These results are presented in Table 2 for each household. The data are reported as both a surface loading (ng/m2) and as a concentration in the dust (ppb) as data have been reported by others using both measures. Previous work suggests surface loading may be better related to possible health effects. Davies et al. (1987) found a better correlation between lead surface loading and hand lead than between lead concentration in dust and hand lead. The correlation between the concentration (ppb) and pesticide loading (ng/m2) measures was significant (at the 99% level) and robust for only two pesticides, chlorothalonil and g-BHC. For the remainder that could be statistically tested, the coefficients were also generally near zero. The total pesticide loading on the floor is understated by these data. First, the large particle size fraction (>150 iim diameter) was separated and was not submitted for analysis. Some pesticide materials may have been present in this segment of the floor dust. Second, the HVS2 does not collect 100% of the dust in a carpet. It is not known what fraction of the dust in the carpet is "available" for human uptake or how this relates to the fraction of dust which is collected by the HVS2. The HVS2 does collect a fraction which is approximately constant with loading and for different carpet materials. An average of 7.5 target pesticides were identified in the indoor air at the nine sites, while an average of 11.8 pesticides were identified in the dust. The number observed in the floor dust ranged from 2 to 23. Thirteen pesticides were found only in the dust in these nine houses. Four of these (PCP, ODD, atrazine, and carbaryl) were not observed in indoor air in any of the samples taken during the Phase III Jacksonville segment of NOPES. In addition, six others (heptachlor epoxide, captan, methoxy- chlor, cis- and trans-permethrin, and DDT) were observed in indoor air of no more than four sites in the entire Jacksonville Phase III study. Conversely, of the six pesticides which were observed in samples from at least eight sites during this pilot study (heptachlor, chlorpyrifos, aldrin, dieldrin, chlordane, and ortho-phenylphenol), all but one were also observed in the air at most of those locations. The exception is aldrin, which was observed in the air at only two sites. A summary of the median value (of the sites where that pesticide was observed) and maximum value for floor dust concentration in ppm and loadings in ng/m2 of the most commonly observed pesticides is provided in Table 3. The relatively fewer number but higher loadings of pesticides observed in four of the households (1064-011, 0966-021, 0782-038, and to a lesser extent 1647- ------- Table 2. Concentration of Pesticides in Surface Dust 1227-216 0753-039 Household DichlorvQs o-Phenylphenol Propoxur Bondiocarb a-BHC HCB Atrazine PCP g-BHC Diazinon Chlorothalonil Carbaryl Heptachlor Malathton Chlorpyrifos Aldrin Dacthal Heptachlor epoxlde Oxychlordane Cap/an Chtofdane Folpet 2.4.D DDE Die/drift DDT ODD Methoxychlor c-Permothrin t-permethrin nglm2 ppb nglm2 399" 60" 8730 1315 5778* 13228 1992 2565" 21 2646" 398" 22 17 254 38 249 76190 11474 17851 3810 574 10 1812 273 19550 600 187 28 1440 4772- roos- ppb 1896" 842" 7 7 5 82 5857 3 6415 197 472 1566" 330" 1064-014 nglm2 22" 464 1" r 635 9 21" 13" 427 55 3* 71 225 19 32 4" I PPb • 360* 7600 13" [ | 10" ^0400 \ 152 340" 216" 7000 I 908 50" ; 7770 ' 3680 306 524 60' 0490-026A nglm2 85* 203" 276* 40* 4* 1111" 255 ' 215" 213" 1984 1894 5758 12" 43 651** 18206 520 414 330" 73" ppb 69* 165" 224* 32* 3" 903" 207 175* 173' 1613 1540 4681 10" 35 529" 14800 423 336 268"* 59" 0490-026B 1440-016A nglm2 433 160* <40 124 5* 167" 3017 594 136* 1095 457* 3150 6947 226 14 187 31218 70 371 5765 1263 372 654 ppb nglm2 1368 171* 505* 167" <100 391 14* 526" 9526 1876 12* 428* <200 3458 12* 1443* 9947 112 21937 260 713 13* 43 589 98584 3655 220 1173 234 18205 176 3988 27 1174 2066 ppb 179* 175" 13* <100 12" 118 273 14* 3838 246 785 28 Notes: " Value less than defined quantitation limit. Value is mojre uncertain than others. Value is more uncertain than others due to continuing calibration drift. < Pesticide confirmed as present in quartz fiber filter or PUF plug but not detected in cyclone due to required for analysis. Value shown is approximately detection limit of cyclone catch sample. Blanks and analytes not listed are not detected or. more properly, "less than detection limit." (Continued) high dilution ------- I Table 2. Continued 1440-016B Household Dichlorvos o-Phenylphenol Propoxur Bendiocarb a-BHC HCB Atrazine POP g-BHC Diazinon Chlorothalonil Carbaryl Heptachlor Malathion Chlorpyrifos Aldrin Dacthal Heptachlor epoxide Oxychlordane Captan Chlordane Folpet 2,4,0 DDE Dieldrin DDT ODD Methoxychlor c-Permethrin t-permethrin nglm2 233* 698 9* 254* 86 357 25 74" 7076 589 254 405 6* ppb 270* 629 8* 229* 77 327 22 67* 6374 530 229 364 6* 7647-007 7064-077 0966-027 0782-038 nglm2 ppb nglm2 ppb ng/m2 <200 <800 <7000 <1000 < 32000 <100 <500 47540* <20 <90 <300 < 7000 57473* <9000 <2000 < 39000 <20 <700 <700 <200 74729* 2073 8226 4437* 947* 59623 263* 7045 7390* 295* 7747* 36* 743 < 79000 7767* 4630 72965* 2753* 783894* <3000 352* 7398 3672* 780* 7433* 8990* 5758* 27477* 26254* ppb nglm2 ppb <7000 7786* 2469* <2000 633* 2564 793657 7747 333* 77270* 67* <800 7908* <700 320" 387* 248* 923* 7729* Notes: * Value less than defined quantitation limit. Value is more uncertain than others. ** Value is more uncertain than others due to continuing calibration drift. < Pesticide confirmed as present in quartz fiber filter or PUF plug but not detected in cyclone due to high dilution required for analysis. Value shown is approximately detection limit of cyclone catch sample. Blanks and analytes not listed are not detected or, more properly, "less than detection limit." 001) illustrates one of the more difficult problems in the analysis of such multi- component samples. In order to measure .the maximum compound, it was necessary to dilute the extract to the point that the effective detection limit was raised above the expected values of many of the other compounds. Some of the pesticides were observed on the quartz fiber filter or the PUF plug in samples from these four households even though the compound was not reported in the (diluted) cyclone catch extract. The concentrations of these pesticides have been reported in Table 2 as less than the detection limit for the cyclone catch plus the observed value on the filters. Conclusions and Recommendations The use of the HVS2 in this nine-home pilot study has shown it to be an effective and efficient way to collect household floor dust samples of sufficient size to permit detailed chemical analysis. Experience with the HVS2 suggested some minor modifications to the device to make it more maneuverable. Additional study should be undertaken to determine the variability of recovery efficiency of the HVS2 with samples of real house dust. The operating procedures and sampling documentation were found to be workable and complete, although additional comments on the availability of a portable hood for use during cleanup should be added. Analytical procedures were generally satisfactory. However, high concentra- tions of pesticides in some samples; required substantial dilution before they ------- Table 3. Summary of Dust and Pesticide Data Analyte Dust <150 nm o-Phenylphenol Propoxur Diazinon Heptachlor Chlorpyrifos Aldrin Chlordane DDT DDE Dieldrin wiec 1.2 g/m2 0.2 ng/m2 0.4 0.2 0.3 5.6 0.3 12.9 0.4 0.5 0.4 nan ; , ; 1 .3 ppm ' 0.6 0.4 : 0.1 4.7 : 0.3 i 6.3 0.4 0.3 0.5 Maxu 169 g/m2 8.7 ng/m2 41.5 57.4 14.7 193.7 11.3 183.9 9.0 0.6 7.4 num -- 1.9 ppm 7.6 10.4 9.9 21.9 1.0 98.6 4.0 1.2 18.2 could be analyzed. As a result, other analytes were diluted below their detection limit. A cleanup procedure should be developed for the cyclone catch that would remove interfering compounds, allowing accurate measure- ment of all the target compounds. Several pesticides were observed that have not been in widespread use for many years. It is not known if these were long-lived residues from earlier indoor applications, recent applications of old pesticide material, or material tracked in from outside areas which were treated in years past. A relationship was observed between the number of pesticides in the samples and the age of the house. No relationship was found with any of the other physical or socio-economic variables. A significant correlation was observed between sur- face loading (e.g., ng/m2) and dust concentration (e.g., ppmb) for only two pesticides. For other pesticides the cor- relation coefficient was generally small as well as not significant. When a pesticide was present in both the air and dust samples, simple statistical tests suggest, with a high degree of confidence, that a relationship may exist between the air concentration and the concentration in the dust for some pesticides. The sample size was not sufficient to quantify the relationship or to identify which pesticides could be so related. A PDF plug filter was necessary for accurate measurement of alpha-BHC, HOB, gamma-BHC, heptachlor, and aldrin. The source of pesticides found on the PUF plug could be either the indoor air drawn through the HVS2 or pesticide material blown off the dust in the cyclone or on the quartz fiber filter. It was not possible to refute either alternative with the data available. A supplemental study did show that j blowoff could occur over time and was a function of vapor pressure, especially over the short term. Further stud^ will be necessary to determine if the PUF plug, or a lower pressure drop Alternative, is necessary to retain these pesticides and other semi- volatile compounds. This work I leaves a number of questions about household exposure to pesticides unanswered. Although this study has demonstrated the presence of a wide variety pf pesticides in household dust in significant concentrations, it is not clear that this rnaterial presents any risk to residents. However, preliminary studies do suggest that the dust- mediated pathway may be a significant route of exposure, especially for very young children. A series of studies should be conducted to determine the sources of these pesticides and the mechanism of [transfer, if any, from the dust to residents. Specifically, 1) longitudinal studies should be made of pesticide application events, 2) studies should be made of surrounding soils to evaluate "track-in" as a source for the pesticide materials, and 3) studies of pesticide materials on residents, or dirt and surrogates' on very young children, should be conducted to determine the amount and manner of transfer from house dust to residents. References Davies, D.J.A., Watt, J.M., Thornton, I. 1987. Lead Levels in Birmingham Dusts and Soils. Sci. Total Environ. 67:177-185. Roberts, J.W. and Ruby, M.G. 1988. Development of a High Volume Surface Sampler for Pesticides in Floor Dust. U.S. Environmental Protection Agency (EPA/600/4-88/036, PB 89-124630). ------- ------- W. 7. Budd, J. W. Roberts, and M. G. Ruby are with Environmetrics, Seattle, WA 89103. Robert G. Lewis is the EPA Project Officer (see below). The complete report, entitled "Field Evaluation of a High Volume Surface Sampler for Pesticides in Floor Dust," (Order No. PB 90-192 006/AS; Cost: $ 17.00, subject to change) will be available only from: National Technical Information Service I 5285 Port Royal Road ' Springfield, VA 22161 Telephone: 703-487-4650 The EPA Prefect Officer can be contacted at: Atmospheric Research and Exposure Assessment Laboratory U.S. Environmental Protection Agency Research Triangle Park NC 27711 United States Environmental 'Rrtitecfion Agency Center for Environmental Research UnfomnatioiJ ; Cincinnati OH 45268 Official Business Penalty for Private Use $300 EPA/600/S3-90/030 ------- |