DistributionofPesticideResiduesWithinHomesinCentralNewYork ... · Whyatt etal.(2002) reported on pesticide exposure from urban residential use during pregnancy by administering questionnaires

Distribution of Pesticide Residues Within Homes in Central New York State

S. K. Obendorf,1 A. T. Lemley,1 A. Hedge,2 A. A. Kline,2 K. Tan,1 T. Dokuchayeva1

1 Department of Textiles and Apparel, College of Human Ecology, Cornell University, Ithaca, New York 148532 Department of Design and Environmental Analysis, College of Human Ecology, Cornell University, Ithaca, New York 14853

Received: 1 September 2004 /Accepted: 19 May 2005

Abstract. Residues for 17 pesticides were analyzed in 41households in central New York State that represented farm,rural, and urban houses. Samples were taken in both summerand winter of 2000–2001 from the same households from fourlocations; family room carpet; adjacent smooth floor; flattabletop surface; and settled dust collected in a Petri dish on atabletop. Pesticide residues were analyzed to identity factorsthat influence both the transport into and the redistribution ofpesticides in the indoor environment. Differences were ob-served between the various pesticides and pesticide classifi-cations relative to location within and between households aswell as by season. Variations in the pesticide residues wererelated to a number of factors. Higher residues were observedin the farm households, particularly in summer, with thehighest amount observed for chloropyrifos in carpet (33 lg/m2). For many pesticides, the frequency of detection and theamount of residues were higher in summer, which relates tousage patterns in agriculture and horticulture; however, largeramounts of insecticides such as mecoprop, resmethrin, andtetramethrin were found on flat surfaces in winter, indicatinghousehold use and possible redistribution within the home.Distribution patterns suggest that routines within a householdmay cause high variation in residues; these practices includeindoor pets and treatment for fleas and ticks, use of termiti-cides, and fastidiousness of occupants. Frequency of pesticidedetection was highest in carpet for both summer and winter forall households, indicating that carpets hold pesticides overtime. Adsorbent fibrous materials such as textiles hold pesti-cides by macro- and micro-occlusion in their complex struc-tures. Amounts of pesticide residue were higher in carpets thanon smooth floors, particularly for rural farm households wherethe farmer was a certified pesticide applicator. The maximumamount of pesticide residue on a smooth floor surface was13.6 lg/m2 malathion while the maxima on wiped surfacesand in settled dust were 1.8 lg/m2 2, 4 D and 3 lg/m2 pen-dimethalin, respectively. Physical properties of individualpesticides such as vapor pressure influenced the distribution of

the pesticide within the households. Evidence of volatilizationof pesticides and redeposition on surfaces was observed,indicating that this is a mechanism for contamination of sur-faces in addition to adsorption on airborne particles andtracking. High residues in winter are evidence that closure ofhouseholds in winter that reduces ventilation results in redis-tribution of pesticides within households.

Pesticides, and in particular organophosphate insecticides, aretoxic compounds that are commonly used both outside andinside U.S. homes. Overexposure to organophosphate pesti-cides and carbamates depresses cholinesterase in red bloodcells, and at a sufficient dose the exposure can be fatal(Tinoco-Ojanguren and Halperin 1998). Moderate pesticideexposure can increase neurological symptoms and elicit cog-nitive and psychomotor dysfunction (Kamel and Hoppin2004). Outdoors, pesticides are subjected to a variety of deg-radation processes, including hydrolysis, biological action, andphotolysis, but indoors, these processes are diminished andpesticides may persist and even accumulate inside buildings(Whitmore et al. 1994). Pesticides may be used inside homesto eliminate insects and they may be tracked into homes fromoutdoor sources on clothing and footwear (Ott and Roberts1998).

Previous studies of indoor pesticides in various regions ofthe United States have shown that residential environments canbe contaminated and many occupants may be exposed topesticides in both urban and rural areas. Whyatt et al. (2002)reported on pesticide exposure from urban residential useduring pregnancy by administering questionnaires to pregnantwomen, and personal air monitoring for a subset of them.Eighty-five percent of the women reported pesticide use in thehome, and all of the women monitored had been exposed todetectable levels of three insecticides and one fungicide. Fourother insecticides were also detected with frequency. Furtherexposure work by Berkowitz et al. (2003) showed throughquestionnaire data that there are high levels (70%) of exposureof urban pregnant women to pesticides, but there were noassociations between these data and urinary metabolites. Es-kenazi et al. (2004) reported on the exposure and effects ofpesticides on Latina women in an agricultural community in

A. A. Kline’s current address is Department of Paper Engineering,Chemical Engineering, and Imaging, Western Michigan University,Kalamazoo, MI 49008, USACorrespondence to: S. K. Obendorf; email: [email protected]

Arch. Environ. Contam. Toxicol. 50, 31–44 (2006)DOI: 10.1007/s00244-004-0185-y

California, While they did not demonstrate adverse effects onfetal growth from exposure, they did find decreases in gesta-tional duration associated with urinary pesticide metabolites.

Curl et al. (2002) studied exposure to organophosphoruspesticides in 218 farm worker households in WashingtonState. They measured metabolites in urine and collected dustsamples. They found significant associations between azin-phosmethyl concentrations in house dust and vehicle dust andwith metabolites from adults and children in the samehousehold. Their results support the hypothesis that the ‘‘take-home exposure pathway contributes to residential pesticidecontamination in agricultural homes where young children arepresent.’’ Other studies report on pesticide residues that haveaccumulated in house dust. Colt et al. (2004) reported geo-graphic variations in pesticide levels in carpet dust samplesfrom 513 homes in Detroit, Iowa, Los Angeles, and Seattlethat were generally consistent with residential pest treatmentpractices. Whitmore et al. (1994) measured total humanexposure to 32 pesticides and pesticide degradation productsin residences located in two urban sites (Jacksonville, FL, andSpringfield/Chicopee, MA) by monitoring 24-h indoor, per-sonal, and outdoor air samples. Indoor and personal air con-centrations of pesticides tended to be higher in Jacksonvillethan in Springfield/Chicopee. Indoor and personal air con-centrations of pesticides were generally comparable and wereusually much higher than outdoor air concentrations. Pesticideconcentrations tended to be highest in summer, lower inspring, and lowest in winter. On average, 12 targeted pesti-cides were found in vacuumed carpet dust in winter comparedwith 7.5 for air samples in the same homes. Also, 13 pesti-cides were found in the carpet dust but not detected in the air.Mean pesticide concentrations in vacuumed carpet dust ran-ged between 0.01 lg g)1 and 15.4 lg g)1. Median carpet dustconcentrations ranged between 0.3 and 6.3 lg g)1. Mean airconcentrations ranged between not detectable and 0.45 lgg)1.

In another Washington state study (Lu et al. 2000) wherespot urine and hand wipe samples were collected from childrenand dust samples were taken, it was found that children ofagricultural workers or who live near treated farmland hadhigher pesticide exposure than other children in the commu-nity. Earlier work on pesticide residues in homes measuredpesticide residues in indoor air, vacuumed carpet dust, outdoorsoil, and on children’s hands (aged 6 months to 5 years) in 9homes (Lewis et al. 1994). The greatest number of pesticidesand highest concentrations were found in vacuumed carpetdust; ingestion of carpet dust may pose the greatest indoorhealth hazard to children (Lewis et al. 1994). In addition,Williams et al. (2003) found that cyfluthrin residue on nyloncarpet was transferred to cotton clothing fabric by rubbing. It isestimated that around two-thirds of residential house dustoriginates from the activities and other processes that occurindoors and one-third from outdoor soil, which is one route foroutdoor pesticides to enter a house (Calabrese and Stanek1992).

The Minnesota Children’s Pesticide Exposure Study(MNCPES) provides exposure data relating to multipathwayexposures of children to four primary pesticides (chlorpyrifos,malathion, diazinon, and atrazine) and 14 secondary pesticides(Clayton et al. 2003). A probability-based sample of 102children aged 3–12 in Minneapolis/St. Paul and in a nearby

rural area (Goodhue and Rice counties) was monitored.Ingestion via solid food rather than beverages or inhalationappeared to be the main intake route for the four primarypesticides, especially for chlorpyrifos, though results were lesscertain for malathion, diazinon, and atrazine because of ahigher number of no detection. The urinary metabolite ofchlorpyrifos showed a stronger association with air measure-ments than with dietary measures. Clayton et al. (2003) foundthat personal-air samples were significantly correlated withindoor air samples for chlorpyrifos, malathion, and diazinon(r = 0.81, 0.51, and 0.62, respectively), and personal-air atra-zine and diazinon levels correlated well with outdoor levels(r = 0.69 and 0.67, respectively). Heightened awareness of thishazard has led to the EPA memorandum of 2000 to prohibitchlorpyrifos end-use product registrations for indoor residen-tial and outdoor non-residential uses (EPA 2000).

As Butt and Heinzow (2002 p. 1) note, ‘‘the role of housedust as an exposure source is gaining more attention...pesti-cides applied outside or within the household that are absorbedand preserved by house dust can lead through the everydayactivities of children and infants to increased exposure. Resi-dential exposure including house dust residues contribute tocombined exposure from dietary and nondietary sources. It isjustified to shift more attention to indoor pollution by housedust contamination and to improve the risk assessment ofnondietary ingestion, but any health-based standard must beaccompanied by a specific dust sampling method.’’

Previous research in central New York State has shown thatmultiple pesticides can be detected in house dust in 10 ruralhomes occupied by certified pesticide applicators and farmers(Lemley et al. 2002). This study extends that work byassessing 17 pesticides in 41 homes in Tompkins and Cortlandcounties in central New York that were surveyed duringsummer 2000 and winter 2001 (Hedge et al. 2002). Thesehomes are equally divided into three categories: farmerhousehold; rural residence not involved with farming; city orsuburban homes. We collected four types of residue: dustsamples collected by vacuuming a designated carpeted area;wipes of hard-floor surfaces (linoleum, tile, or wood); wipes offlat surfaces, such as tables, shelves, or windowsills (non-floorsurfaces); and airborne samples collected on filter paper. Mosthomes contained between 5 and 12 pesticides with the maxi-mum of 15 of the 17 pesticides found in one home. Totalpesticides residues were higher in farm households than innon-farm households, either rural or urban, and the level ofresidue was higher in carpet dust than in dust collected fromsmooth floors. Few differences in numbers of pesticides de-tected were found between seasons or between floor types. Thepurpose of this report is to analyze the distribution of indi-vidual pesticide residues already present within these house-holds in order to identity factors that may influence both thetransport into and redistribution of pesticides in the indoorenvironment. Differences between the various pesticides andpesticide classifications relative to location within and be-tween households as well as by season are identified. Pesticideprofiles developed in this work are related to environmentalfactors including the season, sample location within thehousehold, and the type or category of the household, i.e., ruralfarm, rural non-farm, and urban. Contributions of pesticide usepractices such as agriculture, horticulture, and household pestsare evaluated to determine possible sources of the pesticide

32 S. K. Obendorf et al.

residues. Pesticide use and chemical profiles are used to de-duce transport mechanisms such as tracking and airbornedeposition.

Experimental Procedures

Each of 41 randomly selected homes in central New York Statewas visited during summer and winter for sample collection.This analysis is part of a larger study including sampling forbiological contaminates (Hedge et al. 2002). The samplingprocedures are summarized below. Three categories of house-holds were included: 13 rural farmers (RF), active farmersincluding those who were certified pesticide applicators; 14rural homes (RH), in which the residents were not involved withfarming; 14 urban houses (UH), city or suburban home. Testspecimens were collected at four locations within each house-hold: smooth floor (BF) and carpet (C) areas in the family livingroom, the surface of flat tabletop surface (FS), and settled dustcollected in a Petri dish on a tabletop (Dust). Summer speci-mens were collected between August and October in 2000,while winter specimens were collected from January throughMarch in 2001. Data were calculated in mass per unit area (lg/m2). On the first visit to each house, two Petri dishes, each witha Whatmann filter paper inside, were placed on a surface, suchas a shelf, and left exposed to the air for a one-week period. Thesettled dust samples were collected on the second house visit.The dust that settled on the filter paper was analyzed. Data fromthe second visit are used in this analysis. Each house was visitedtwice. At the first visit, the carpet, floor, and shelf areas werecleaned and Petri dishes for settled dust were put in place.Occupants were asked not to clean these surfaces until after thenext visit. One week later, a second visit was made and thecarpet was vacuumed, the bare floor and flat surfaces werewiped, and the settled dust samples were collected. In this way,there was a constant time interval for all samples.

The vacuum samples were collected using a new, com-mercially available motorized vacuum cleaner (Hoover WindTunnel) fitted with a microfiltration vacuum bag (99.7%capture at ‡1 lm). The use of this vacuum cleaner for sam-pling emulates what occurs domestically in the houses. Thisvacuuming method compares well with dust samples obtainedusing specialized vacuum cleaners, such as the HSV-3 (e.g.,Lewis et al. 1994) and it has been validated as a reliablemethod for pesticide sampling (Colt et al. 1998). In the living/family room, a designated carpet area was measured and re-corded. The area varied between homes and depended on theroom size. A new microfiltration vacuum bag was used foreach sample visit to each house, and the vacuum was cleanedafter each sample by thoroughly wiping and swilling allpathways with a 70/30 (by volume) mixture of methanol anddistilled water. The efficacy of this cleaning method was testedin the laboratory prior to field deployment of the vacuumcleaner. The designated carpet area was vacuumed using themotorized self-drive mechanism of the vacuum, with fourcomplete forwards-backwards passes, two in one direction,then two in the orthogonal direction. Once completed, thevacuum bag was removed, sealed and placed in a sealed plasticcontainer, put on ice, and transported to the laboratory, whereit was stored in a freezer until analysis.

The smooth floor dust was collected by hand wiping ameasured smooth floor area (�0.372 m2) with 4 strokes (leftand right, back and forth) using a Whatmann filter paperwetted with a 70/30 (by volume) mixture of methanol anddistilled water. The wipe was placed in a sealed glass con-tainer, put on ice, and transported to the laboratory, where itwas stored in a freezer until analysis.

Samples from flat surfaces, such as tables, shelves, orwindowsills, were taken using a Whatmann filter paper thathad been wetted with a 70/30 (by volume) mixture of methanoland distilled water and wiping a measured area in two direc-tions. The wipe was placed in a sealed glass container, put onice, and transported to the laboratory, where it was stored in afreezer until analysis.

On the first visit, the Petri dishes for settled dust collectionwere placed, after the carpet had been vacuumed, on surfacesin the room where they would not be disturbed by people ordogs between visits, such as on a shelf, and left exposed to theair for a one-week period. The samples were collected on thesecond house visit. Collection involved putting the filter paperin a jar and rinsing out the Petri dish into the sample glass jarwith the 70/30 water/methanol mixture that contained the filterpaper. The sample glass jar was then covered, sealed, put onice, and transported to the laboratory, where it was stored in afreezer until analysis.

Pesticide Analyses

Seventeen pesticides were extracted and analyzed as wipe ordust samples using methods developed specifically for thisproject (Hong et al. 2001) (Tables 1 and 2). The pesticides,exclusive of degradation products, were monitored. The non-acid pesticides were methamidophos, carbaryl, atrazine, me-thyl parathion, alachlor, pendimethalin, metolachlor, diazinon,malathion, tetramethrin, trifluralin, resmethrin, and chlorpyri-fos. The acid pesticides were picloram, 2, 4-D-acid, dicamba,and mecoprop.

The non-acid pesticides were first extracted from dust withethyl acetate: cyclohexane (3:1) which was replaced with di-chloromethane. The extract was filtered and collected for fur-ther cleanup with Size Exclusion Chromatography (SEC) usinga high-resolution SEC polyvinyl benzene/polystyrene column(EnvirosepABC column) protected by an EnvirosepABC guardcolumn (Phenomenex, Torrance, CA) on a HP1090 HPLC(Agilent Technologies, Sunniyvale, CA) equipped with diodearray detector (DAD). Detailed SEC conditions can be found inHong et al. (2001). The effluent was collected manually andcondensed for GC/MS analysis. Filter paper samples were ex-tracted with acetone for GC/MSD analysis. Pesticides wereanalyzed on a HP5890 Series II gas chromatograph coupled to aHP 5971A MS (Agilent Technologies, Sunnyvale, CA).Operating conditions are detailed in Hong et al. (2001). Pesti-cides were identified by matching both characteristic MSfragment ions and chromatographic retention times.

Acid pesticides were extracted three times from dust withdistilled water and Ca(OH)2 (weight ratio of dust: Ca(OH)2

was adjusted to 1:0.1). The pH was adjusted to 1 to 2 and theeffluent was cleaned up by SPE with a polyvinylbenzene/polystyrene cartridge (Oasis HLB 6 mL, Waters Co. Milford,MA). The cartridge was washed with distilled water at pH 2

Pesticide Residues in Homes in New York State 33

and eluted with methanol in MTBE. The solution was ex-tracted with diethyl ether and dried, followed by addition ofmethanol and trimethylsilyl diazomethane to methylate thecarboxylic acid pesticides.

Filter paper samples were extracted with acidified acetone(3 mM H3PO4). The extract was condensed, methylated, andinjected into the GC in the same way as dust extract exceptSPE cleanup was not used. Optimized GC/MS conditions weresimilar to those for non-acid pesticides (Hong et al. 2001).

Statistical Analyses

Pesticide data were analyzed with logistic regression to studythe detection of residue within the households. In order toexamine the main effects and interaction effects of all inde-pendent variables on the dependent variable-pesticides counts,Multiway Analysis of Variance (ANOVA), mixed modelanalyses with house-id as the random effect, were performedon the non-zero pesticides data using the SAS program (SASInstitute Inc., Cary, NC). Based upon the residual plots, atransformation of log (counts+0.00001) was applied to assurethat the data conformed to the assumptions underlying ANO-VA. Effects were tested for significance at the 0.05-alpha le-vel.

Results and Discussion

Previous analysis by Hedge et al. (2002) found that the totalpesticide residue varied with type of household (category) andthe location and type of surface (floor) with higher amountsfound on carpets compared to smooth surfaces. They alsofound the expected seasonal difference between summer andwinter for pesticide residue in the household with higher levelsof pesticide residue and more pesticides observed in thesummer. In this work, we do further analysis of frequency ofdetection and amount of residue for individual pesticides,finding that main effects of floor/surface type, householdcategory, and pesticides were significant for both frequency ofdetection and amount of residue (Table 3).

Main Effects

Interestingly, season was significant as a main effect for fre-quency of detection, with pesticides being more frequentlydetected in summer, but when only the non-zero data wereincluded in the ANOVA, season as a main effect was notsignificant. The number of households in which we detectedresidue was higher in summer for nine pesticides, most ofwhich are used in agriculture or in agriculture and horticulture.Tetramethrin, an insecticide used in the home and garden, wasalso observed in more households on all surfaces duringsummer. Seasonal differences varied with pesticide and withthe category of households. Larger seasonal differences wereobserved for rural farm households.

The most frequently detected pesticide during summer onflat surfaces and smooth floor was diazinon, an insecticideused in home, garden, and pet applications as well as agri-

culture. The highest amount of pesticide residue was observedin summer for malathion on all of the four surfaces evaluated.Other pesticides for which high amounts were detected insummer are chlorpyrifos in carpet dust, dicamba in settleddust, methamidophos on smooth floor, and, 2, 4 D on the flatsurface.

Differences were observed between pesticide usage classi-fications, i.e., agriculture, agriculture and horticulture, andhousehold (Table 3). Pesticides in the use classifications thatinclude agriculture (Table 2) were present in higher amounts(agriculture 1.1 lg/m2, agriculture and horticulture 1.2 lg/m2)than the pesticides classified for household use (0.4 lg/m2).Their frequency of detection also was three times higher.These results are in agreement with research by Fenske et al.(2000) who pointed out higher pesticide exposures of familiesof agricultural workers.

Two- and Three-Way Interactions

In addition to differences in main effects, the logistic regres-sion and ANOVA showed significant two- and three-wayinteractions (Table 3). Two-way interactions of floor · cate-gory and season · pesticide were significant for both fre-quency of detection and amount of residue, and theinteractions of floor · pesticide, season · floor, and category ·pesticide were significant for amount of residue. To furtherunderstand these data with high numbers of no detection andsignificant two- and three-way interactions, we used a logisticregression to investigate the detection of the pesticides, fol-lowed by an analysis of variance using only the non-zero datacalculated separately for surface types (carpet, smooth floor,flat surface, settled dust) (Tables 4–7).

Differences in the frequency of detection of pesticide resi-due by household category, i.e., rural farmer (RF), rural non-farming (RH), and city/suburban (UH), were observed foratrazine, chloropyriphos, diazinon, and trifluralin in carpetdust (Table 4), for malathion on smooth floor (Table 5), andfor chloropyrifos in settled dust (Table 7). Higher amounts ofresidue were found in carpets of rural farmer household foralachlor, 2, 4-D, diazinon, dicamba, mecoprop, methamido-phos, and picloram. All of these are used in agriculture, andsome are also used in horticulture. The overall maximumresidue observed was for chloropyrifos (33.1 lg/m2), aninsecticide used in agriculture, horticulture, and the home. Thismaximum was found in summer in carpet dust in a rural farmerhousehold (RF) of a licensed applicator. A relatively highmaximum (30.8 lg/m2) was also observed for malathion, an-other insecticide. This maximum was also observed in thesummer in carpet dust but in a rural household in which theoccupant was not involved in farming, The lowest maximumamount on carpet (1.5 lg/m2) was for dicamba, an herbicideused in agriculture (Table 4).

Floor Types

The largest F value and Chi square were for floor type (Ta-ble 3). Pesticides were more frequently detected on carpets,and pesticide levels were significantly higher in carpet dust


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than in the other surfaces evaluated (Fig. 1) as reported byHedge et al. (2002). The highest frequency of detection was oncarpets in rural farmer households in summer. One reason forthis result is the fibrous nature of the carpet which has a veryhigh fiber surface area for adsorption of pesticides. Another isthe complex textile structure that will retain particles bymacro- and micro-occlusion in fiber interstices and irregular-ities. Carpet and settled dust specimens were both collected onfibrous surfaces. We expressed the data for pesticide residue asmass per area of the household object; for the carpet, there is amuch larger fiber surface area. This could explain why theresidue maxima for the 17 pesticides were observed inthe carpet samples (Table 4). Lewis et al. (1994) found that thegreatest number and highest amounts of pesticides were foundin carpet dust, possibly arising from indoor treatments or bytrack-in from the outdoors. Similarly, Whitmore et al. (1994)found that 12 pesticides were found in carpets compared to 7.5in air samples collected in the same nine residences.

Differences in frequency of detection in the carpet betweentypes of households were found for atrazine, diazinon, andtrifluralin; these pesticides were found more frequently inhouseholds of rural farmers (RF) than in urban households(UH). Amounts of residue in carpets for rural farm householdwere also higher than for non-farm households for alachlor, 2,4D, diazinon, dicamba, mecoprop, methamidophos, and piclo-ram.

Carpets had much more residue than the smooth floor andflat surfaces (Fig. 1); these differences were significant for allpesticides except methamidophos and tetramethrin, both ofwhich were found in higher amounts on smooth floor. Amount

of residue did not differ significantly for dicamba and pendi-methalin; these pesticides were present in very low amounts,< 1 lg/m2. Malathion and chloropyrifos, organophosphateinsecticides, were observed on carpets in higher amounts thanon the other surfaces analyzed (smooth floor, flat surface,settled dust). This could relate to household use of theseinsecticides to control mosquitoes, fleas and ticks, cock-roaches, silverfish, ants, and termites both within the structureand in the garden. Two herbicides, alachlor and metolachlor,were also found in carpet dust at levels above 2 lg/m2.

In general, smooth floor and flat surface samples had loweramounts of pesticide residue (<3 lg/m2) than that observed forcarpets (up to 32 lg/m2). Those pesticides found at high levelsfor both carpet and smooth floors are malathion and methami-dophos. Smooth floor had higher residue amounts of thesepesticides than non-floor surfaces (flat surface and settled dust)for 13 out of the 17 pesticides, with the highest amount observedfor methamidophos, malathion, and metolachlor (Fig. 2). Thesetwo insecticides and one herbicide, metolachlor, used on agri-cultural crops, were present at levels above 1 lg/m2. The factthat smooth floor residues were higher than the non-floor sur-faces appears to be evidence that pesticides are tracked into thehousehold on shoes and feet of occupants and possibly pets.Diazonin was the most frequently detected on both the smoothfloor and flat surface. Chloropyrifos was found in significantamounts, and for one household we observed a residue level of9.9 lg/m2. The average residue of tetramethrin was similar tothat of chloropyrifos, but was observed more frequently (35households) and at lower levels, with the maximum observedbeing 1.6 lg/m2.

Table 2. Pesticide classification and use (Tomlin 1997)

Use Pest Pesticide Crop

I. Agriculture A. Herbicide Alachlor Field corn, soybeans, and peanutsAtrazinea Corn, sorghum, sugarcane, pineapple, Christmas trees, forestsDicamba Grain crops and grasslands, fence-rows and roadwaysMetolachlor Field corn, soybeans, peanuts, grain sorghum, potatoes,

pod crops, cotton, safflower, stone fruits, nut trees,highway rights-of-way, and woody ornamentals

Piclorama Control of woody plants and a wide range of broad-leaved weeds, range landPendimethalin Field corn, potatoes, rice, cotton, soybeans, tobacco, peanuts, and sunflowersTrifluralin Tree fruit, nut, vegetable, and grain crops, including soybeans, sunflowers,

cotton, and alfalfaB. Insecticide Methamidophos Potatoes, tomatoes, cotton, alfalfa

Methyl parathion Agricultural crops, primarily on cottonII. Agriculture

and horticultureA. Herbicide 2, 4-D Pasture and rangeland, home, garden, and aquatic

Mecoprop Ornamentals and sports turf, forest, drainage ditch banks, wheat, barley, and oatB. Insecticide Carbaryl Citrus, fruit, cotton, forests, lawns, nuts, ornamentals, shade trees, and other crops,

as well as on poultry, livestock, and petsChlorpyrifos Grain, cotton, corn, fruit, nut and vegetable crops, lawns and ornamental plants as

well as sheep and turkeys, horse, dog kennels, domestic dwellings, farm buildings,storage bins, and commercial establishments

Diazinona Residential, non-food buildings, home gardens and farms, fruit trees, sugarcane, corn,tobacco, potatoes, horticultural plants, veterinary uses against fleas and ticks

Malathion Fruits and vegetables, and householdIII. Household B. Insecticide Resmethrina Greenhouses, indoor landscapes, mushroom houses, industrial sites, stored products,

fabric protection, pets, and horsesTetramethrin Public, home and garden, indoor spaces

a Restricted-use pesticide.


Methamidophos was the pesticide with the highest residueon the smooth floor. Since this pesticide has a vapor pressureof 4.7 mPa (Table 1), one of the higher vapor pressures in thegroup studied, we questioned the role of volatilization in thedistribution of pesticides within the households. Vapor pres-sures for the other pesticides ranged from 0.0015 to 13.7 mPa.All of the pesticides that we analyzed were liquid or solid atroom or ambient temperature. This suggests that one mecha-nism of contamination might be evaporation of pesticides,which could redistribute pesticides such as methamidophos onsurfaces within the households. This hypothesis was investi-gated further in our discussion of residues in settled dust versusflat surfaces (vide infra).

Pesticide residues observed on the smooth floor surface alsovaried by type of household. Malathion was more frequentlydetected on these surfaces for rural farm households (RF) andleast frequently in city suburban households (UH). Residues onsmooth floors varied with season, with 8 pesticides being morefrequently detected in summer (atrazine, 2, 4 D, diazinon,mecoprop, methamidophos, methyl parathion, metolachlor,and tetramethrin). These seasonal differences seem reasonabledue to the use patterns for these pesticides during the growingseason. Resmethrin was detected on the smooth floor morefrequently in winter than summer, and, when detected, theresidues for alachlor, 2, 4 D, and tetramethrin were higher inwinter than summer. This observation may indicate a redis-

Table 3. Logistic regression for all data and ANOVA for non-zero data

Logistic regression ANOVA

Effect Degrees of freedom Chi square Pr>Chi square F value Pr > F

Season 1 26.29 <0.0001 0.2 0.6651Floor (and surface type) 3 32.93 <0.0001 20.2 <0.0001Category 2 6.29 0.0432 14.1 <0.0001Use 2 10.03 0.0066 12.4 <0.0001Pesticides 14 33.59 0.0024 13.9 <0.0001Season · floor 3 2.48 0.4788 20.6 <0.0001Season · category 2 4.80 0.0906 1.1 0.3302Season · use 2 0.74 0.6921 11.2 <0.0001Season · pesticide 14 27.98 0.0143 4.6 <0.0001Floor · category 6 19.00 0.0042 10.4 <0.0001Floor · use 6 8.33 0.2146 1.9 0.0757Floor · pesticide 42 42.00 0.4710 5.0 <0.0001Category · use 4 14.72 0.0053 1.7 0.1390Category · pesticide 28 25.40 0.6058 4.3 <0.0001Season · floor · category 6 12.93 0.0442 3.6 0.0017Season · floor · use 6 6.90 0.3298 3.6 0.0014Season · category · use 4 6.71 0.1517 1.1 0.3268Floor · category · use 12 10.01 0.6155 0.9 0.5482

Table 4. Logistic regression and ANOVA for carpet

PesticideMinimum(lg/m2)

Maximum(lg/m2)

Logistic categorydetection Pr

ANOVA categoryamount Pr

Logistic seasondetection Pr

ANOVA seasonamount Pr

Alachlor 0.005 18.1 0.2614 <0.0001 0.1537 0.0030Atrazine 0.011 7.7 0.0006 0.1092 0.0033 0.9875Carbaryl 0.148 3.2 0.0904 0.0604 0.3849 0.1378Chlorpyrifos 0.226 33.1 0.0314 0.1423 <0.0001 0.00792, 4 D 0.010 4.6 0.4774 <0.0001 0.1603 0.0013Diazinon 0.006 8.0 0.0131 0.0064 0.0244 0.0021Dicamba 0.001 1.5 0.3963 <0.0001 0.1501 0.1983Malathion 0.451 30.8 0.0609 0.2087 <0.0001 0.0458Mecoprop 0.001 3.2 0.6684 <0.0001 0.0356 0.8505Methamidophos 0.063 9.4 0.2137 0.0197 0.0101 0.0022Methyl parathion 1.236 4.1 0.7566 0.5476 ne neMetolachlor 0.062 5.9 0.9596 0.0992 0.0080 0.0025Picloram 0.002 9.5 0.0632 <0.0001 0.7918 0.0057Pendimethalin 0.043 5.2 0.0928 0.7186 0.1708 0.8995Resmethrin 0.025 6.3 0.0768 0.0148 0.0234 0.6833Tetramethrin 0.008 3.7 0.2940 0.1669 0.0007 0.0424Trifluralin 0.033 8.7 0.0148 0.2225 0.4570 0.5422

ne, nonestimable.


tribution of chemicals within the household during the winterseason when the windows are closed and there is evaporationand/or aeration of particles by mechanical action such aswalking and use of the vacuum cleaner.

Smooth Surfaces

The pattern of frequency of detection and residue amounts issimilar for the flat tabletop surfaces and the smooth floor

Table 6. Logistic regression and ANOVA for flat surface


Maximum(lg/m2)





Alachlor 0.023 0.9 0.6234 0.1291 0.0368 0.4340Atrazine 0.022 0.7 0.9822 0.4918 0.5468 0.1951Carbaryl 0.040 1.5 0.4400 0.0353 0.7447 0.8383Chlorpyrifos 0.023 0.4 0.9591 0.7852 0.9707 0.10292, 4 Da 0.022 1.8 0.2087 0.9957 0.0013 <0.0001Diazinon 0.008 0.8 0.2142 0.7835 0.0010 0.4217Dicamba 0.002 0.8 0.7949 0.9601 ne neMalathionb 0.002 1.3 0.2104 0.9593 0.6960 <0.0001Mecoprop 0.001 0.5 0.1225 0.3297 0.3986 0.0080Methamidophos 0.078 1.1 0.0842 0.1437 0.0114 0.8613Methyl parathion 0.235 0.9 0.5304 0.9992 0.1940 0.7047Metolachlor 0.146 1.0 0.8983 0.0142 0.2579 0.3657Picloram 0.004 1.0 0.0980 0.4853 0.0041 0.2028Pendimethalin 0.013 0.8 0.5593 0.2927 0.5604 0.0553Resmethrin 0.001 0.9 0.1013 0.2504 0.4596 0.0366Tetramethrinc 0.003 0.8 0.2697 0.0724 0.0906 0.0974Trifluralin 0.006 0.5 0.9486 0.1775 0.3913 0.5576

ne, nonestimable.a Anova 2, 4 D category · season <0.0001.b Anova malathion category · season <0.0001.c Anova tetramethrin category · season 0.0054.

Table 5. Logistic regression and ANOVA for smooth floor


Maximum(lg/m2)





Alachlora 0.002 2.9 0.9128 0.0005 0.7253 0.0003Atrazine 0.003 1.0 0.2226 0.1190 <0.0001 0.3529Carbaryl 0.013 3.6 0.1255 0.8686 0.8424 0.9375Chlorpyrifos 0.244 9.9 0.7240 0.3503 0.7285 0.67172, 4 D 0.006 0.8 0.1830 0.6148 0.0161 0.0010Diazinon 0.001 1.7 0.2334 0.6686 <0.0001 0.9766Dicamba 0.001 0.5 0.4042 0.6122 0.0051 0.1504Malathionb 0.035 13.6 0.0044 0.9021 0.2304 0.8401Mecoprop 0.001 4.4 0.1197 0.6193 0.0128 0.0126Methamidophosc 0.001 7.8 0.9790 0.0391 0.0442 0.0643Methyl parathion 0.236 1.2 0.6812 0.2232 0.0542 0.0505Metolachlor 0.694 1.9 0.5075 0.1757 0.0333 0.1391Picloramd 0.004 1.6 0.1879 0.1368 0.0523 0.7625Pendimethalin 0.006 1.1 0.9998 0.8462 0.2503 0.7470Resmethrin 0.001 1.4 0.2282 0.5596 0.0484 0.0162Tetramethrine 0.001 1.6 0.5420 0.4011 0.0003 0.0113Trifluralin 0.012 1.3 0.6570 0.4100 0.3561 0.1360

a Anova alachlor category · season 0.0008.b Logistic malathion category · season 0.0412.c Anova methamidophos category · season 0.0081.d Anova picloram category · season 0.0009.e nova tetramethrin category · season 0.0096.


(Figs. 2–4). For example, diazinon is the most frequently ob-served pesticide for both of these surfaces. Similar amounts ofresidue were found for several of the pesticides on these twosurfaces. These relationships suggest airborne deposition ofpesticides. Pesticides that were found on flat surfaces morefrequently in summer are alachlor, 2,4 D, diazinon, metham-idophos, and picloram. Difference between household cate-gories was found for metolachlor, which was found in largeramounts in rural households (RH). Malathion was found inlarger amounts on flat surfaces in summer. Winter amountswere higher for 2, 4 D, mecoprop, and resmethrin. Frequenciesof detections were similar for all household categories for eachof the pesticides, and the amounts of residue were also similar,with only metachlor residue being higher for rural households(RH), Frequency of detection of diazinon was much higher insummer. There were statistically higher frequencies of detec-tion also for alachlor, 2, 4 D, methamidophos, and picloram insummer (Table 6). Residues on flat surfaces were higher insummer for malathion, while 2, 4 D, mecoprop, and resmethrinresidues were all higher in winter.

Average pesticide residues on flat surfaces were all below1.1 lg/m2, with the overall maximum value observed for 2, 4D of 1.8 lg/m2. These residues could be deposited from theair, either by volatilization or adsorption on airborne particles.Pendamethalin was the most frequently observed pesticide insettled dust, and the maximum observed in any household was3 lg/m2. For settled dust, the pesticides with the highestamounts of residue are dicamba (4.5 mPa), malathion (5.3mPa), trifluralin (6.1–13.7 mPa), and chloropyrofos (2.7 mPa),all of which have vapor pressures at the high end of the range(Table 1). This provides some evidence that volatilization ofpesticides is another mechanism for surface contaminationwithin the households in addition to adsorption on airborneparticles.

Settled Dust

Two pesticides, chloropryifos and malathion, were present inlarge amounts in settled dust; it is interesting that they are alsopresent in large amounts in carpet dust. It could be that theyare redistributed from the carpet dust. Diazinon, an insecticideused in domestic households in pest strips and for control offleas and ticks on pets, was found in settled dust more fre-quently and in larger amounts in rural and urban householdsthan in farm households. Dicamba, an herbicide used for broadleaf weed control, was found in settled dust in larger amountsin rural farm households.

Settled dust residues were distinctly different from flat sur-faces for several pesticides (Fig. 5). It was an objective of thestudy to determine the extent of deposition from the air as amechanism for contamination. Filter paper was used as thecollection medium. The amount of pesticide residue per m2 offilter paper in the Petri dish was high relative to that found onthe flat surface, a curious result since one might expect thesesurfaces to be contaminated by similar mechanisms. If thepesticide is evaporated due to a high vapor pressure and thenadsorbed onto the filter paper, one would expect a higheramount to be adsorbed onto the fibrous substrate of the filterpaper than on a hard surface due to the very high fiber surfacearea per area of the filter paper. Much higher amounts of pes-ticide were observed on the filter paper collection medium(settled dust) for chloropyrifos, dicamba, and trifluralin. Theseare semi-volatile pesticides with vapor pressures of 2.7, 4.5,and 6.1–13.7 mPa, respectively. This suggests that settled dustis the result of deposition by more than one mechanism.

To further understand the data called ‘‘settled’’ dust, wedid an experiment. We wanted to know if a volatilized pes-ticide would be adsorbed on a hard surface, e.g., plastic, andon a fiber surface, e.g., filter papers in a closed environment.

Table 7. Logistic regression and ANOVA for settled dust


Maximum(lg/m2)





Alachlor 0.011 1.5 0.8278 0.6578 0.8487 0.5672Atrazine 0.010 0.5 0.3906 0.0055 0.5628 0.0093Carbaryla 0.006 1.0 0.3613 0.0217 0.0666 0.0044Chlorpyrifos 0.001 1.7 0.0226 0.3322 0.8672 0.10072, 4 D 0.007 1.5 0.7478 0.2657 0.0513 0.3558Diazinonb 0.016 2.0 0.6201 0.3415 0.0444 0.8819Dicamba 0.044 2.5 0.8032 0.5226 0.9988 neMalathion 0.008 2.0 0.6186 0.1035 0.4161 0.2649Mecoprop 0.002 0.4 0.7303 0.5355 0.6642 0.5084Methamidophos 0.006 0.4 0.6801 0.1955 0.3255 0.2443Methyl parathionc 0.125 0.125 ne ne ne neMetolachlor 0.301 0.8 ne 0.3514 0.1782 0.5533Picloram 0.001 1.2 0.8183 0.9640 0.5919 0.2723Pendimethalin 0.001 3.0 0.0862 0.8391 0.5496 0.4540Resmethrin 0.013 0.8 0.0588 0.0058 0.8965 0.0001Tetramethrin 0.018 0.4 0.2658 0.0107 0.0020 0.6345Trifluralin 0.175 1.8 ne 0.8198 0.3174 0.7171

ne, nonestimable.a Carbaryl category · season 0.0248.b Diazinon category · season 0.0012.c Methyl parathion was detected in only one household (RH) in the winter.


We also wanted to know if the filter paper would adsorbmore pesticide due to the high amount of fiber surface areacompared to the surface area of a hard plastic surface. APetri dish containing 6 g of pesticide with 37.4% pendi-methalin (2.24 g) was placed in a sealed desiccator with anuncontaminated plastic strip and a filter paper strip of equalarea (57 cm2). Six specimens of plastic and filter paper wereexposed to the vapor of pendimethalin for 10 days, afterwhich each specimen was extracted and analyzed in the sameway as the household residues. Pendimethalin was detectedon all samples, indicating contamination by volatilization,and the amount of pendimethalin was five times higher forthe filter paper (0.1 lg/cm2) than the plastic specimen(0.02 lg/cm2). This experiment helps explain the results withthe two fibrous media (carpet and settled dust) compared tothe two hard surfaces (flat table surface and smooth floor). Itsuggests that the higher level of pesticide residue on thesettled dust on the filter paper compared to the flat surface isdue to volatilization of the pesticide within the household(Fig. 5). This mechanism can be more important in the winterwhen the windows and doors are closed compared to thesummer when the windows would be open. Gurunathan et al.(1998) found that chlorpyrifos, a semi-volatile compound,partitioned between the vapor phase and condensed phase,

resulting in a fraction of the pesticide being released into thegas phase and then deposited on other surfaces such aschildren’s toys, residential surfaces, and other sorbent mate-rials, e.g., textile materials. Early research by Fenske et al.(1991) pointed out the importance of ventilation relative topesticide exposures in households.

Contamination of the filter paper medium through thedeposition of particles on which pesticide is adsorbed is be-lieved to have occurred in our study since the extracts of thefilter paper were turbid and gray in color. Some pesticides,such as chlorpyrifos, are strongly adsorbed on soil particles,e.g., clay. Thus, we believe that the measurements that wemade of settled dust on the filter paper in the Petri dishes hadpesticide that was deposited there by both evaporation andairborne particles on which pesticide was adsorbed. In a studyof the distribution of pesticides in house dust as a function ofparticle size, Lewis et al. (1999) found that the concentrationof nearly all target analytes increased with decreasing particlesize with dramatic differences for the smallest particle sizes.Thus, we think that the semi-volatile pesticides, in particular,could be adsorbed on the surfaces of particles and fibers andcould easily redistribute within the household.

Pendimethalin was one of most frequently detected pesti-cides in settled dust. Frequency of detection was higher insummer than in winter for diazinon and tetramethrin, as well asfor chloropyrofos and resmethrin for non-farm households (RHand UH). Larger amounts of residue were found in summerthan winter for carbaryl, while atrazine and resmethrin werehigher in winter. Resmethrin, a household insecticide used forindoor pest control (Table 2), was found in larger amounts innon-farm households (RH and UH). Chloropyrifos was foundmore frequently and in larger amounts in urban households(UH). This is strong evidence of the influence of householduse of pesticides on residue levels in homes. High detectionfrequency and residue amounts in winter support the idea thatchemicals are redistributed within the household by evapora-tion or mechanical action such as a vacuum cleaner that resultsin redeposition. For example, pesticides held in carpets forlong periods of time can become airborne and redistribute ontohousehold surfaces.

Fig. 1. Frequency of pesticide detection (N = 81) and amount ofpesticide residue by household surface

Fig. 2. Comparison of pesticide residue for smooth floor versus flattabletop surface


Fig. 3. Frequency of detection of pesticides and average amount of residue when detected in rural farm, rural, and urban households


Fig. 4. Frequency of detection of pesticides and average amount of residue when detected in summer and winter


Conclusions

Higher residues of individual pesticides were observed forthose pesticides used in agricultural and horticultural applica-tion with the highest residues in summer in rural farm house-holds, especially those of certified pesticide applicators.Residues detected within all of the homes were higher on car-pets than on the smooth surfaces or settled dust, indicating thatcomplex textile structures and high surface areas hold residueover time. In addition, the flat surface samples and the settleddust samples indicate that pesticides that enter the householdsare redistributed within the households by airborne routes. Theresidues indicate that these semi-volatile compounds volatizewithin the households, contaminating surfaces and objects inaddition to becoming airborne by adsorption on small dustparticles. Gas sampling in the household would have provideduseful data. The maximum amount of pesticide residue oncarpet was chloropyrifos at 33 lg/m2, while on smooth floorsurface the maximum was 13.6 lg/m2 malathion, for settleddust it was 3 lg/m2 of pendimethalin, and for a flat surface itwas 1.8 lg/m2 of 2, 4 D, all pesticides used in agriculture.

There is evidence of pest control product use within thehousehold that leads to residues of pesticides on commonsurfaces. Pesticide residues were observed from use of insec-ticides not related to agriculture within households. In general,residues from these practices tend to be lower in both fre-quency and amounts than those used in agriculture and horti-culture. The highest residue found was for cholorpyrifos incarpet, a pesticide used both in agriculture and in dwellings forpest control. Insecticides such as resmethrin and chloropyrifos,used for indoor pest control, were found in larger amounts innon-farm households. There is evidence of the influence ofhousehold use of pesticides on residue levels in homes. Fre-quency and residue amounts in winter support the idea thatchemicals are redistributed within the household by evapora-tion or mechanical action such as a vacuum cleaner. It wouldbe informative to study the presence and storage of chemicalswithin the household. As well, retention and release of pesti-cides from carpets merit further and more careful study.

Acknowledgments. This research was supported in part by the Cor-nell University Agricultural Experiment Station federal formula

funds, Projects No, NYC327402, 329423, and 329478 received fromCooperative State Research, Education, and Extension Service, U.S.Department of Agriculture, and by a grant from the Carpet and RugInstitute. We thank A. Achecar, M. Ames, C. Coffman, V. Gaskins, D.Heath, and T. Miller for their assistance with this work. Particularappreciation is given to FranÅpoise Vermeylen for advice and assis-tance on the statistical analyses.

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