Volatilization of polycyclic aromatic hydrocarbons from coal-tar-sealed pavement.

Coal-tar-based pavement sealants, a major source of PAHs to urban water bodies, are a potential source of volatile PAHs to the atmosphere. An initial assessment of volatilization of PAHs from coal-tar-sealed pavement is presented here in which we measured summertime gas-phase PAH concentrations 0.03 m and 1.28 m above the pavement surface of seven sealed (six with coal-tar-based sealant and one with asphalt-based sealant) and three unsealed (two asphalt and one concrete) parking lots in central Texas. PAHs also were measured in parking lot dust. The geometric mean concentration of the sum of eight frequently detected PAHs (ΣPAH(8)) in the 0.03-m samples above sealed lots (1320 ng m(-3)) during the hottest part of the day was 20 times greater than that above unsealed lots (66.5 ng m(-3)). The geometric mean concentration in the 1.28-m samples above sealed lots (138 ng m(-3)) was five times greater than above unsealed lots (26.0 ng m(-3)). Estimated PAH flux from the sealed lots was 60 times greater than that from unsealed lots (geometric means of 88 and 1.4 µg m(-2) h(-1), respectively). Although the data set presented here is small, the much higher estimated fluxes from sealed pavement than from unsealed pavement indicate that coal-tar-based sealants are emitting PAHs to urban air at high rates compared to other paved surfaces.

Influence of coal-tar sealcoat and other carbonaceous materials on polycyclic aromatic hydrocarbon loading in an urban watershed.

Carbonaceous material (CM) particles are the principal vectors transporting polycyclic aromatic hydrocarbons (PAHs) into urban waters via runoff; however, characteristics of CM particles in urban watersheds and their relative contributions to PAH contamination remain unclear. Our objectives were to identify the sources and distribution of CM particles in an urban watershed and to determine the types of CMs that were the dominant sources of PAHs in the lake and stream sediments. Samples of soils, parking lot and street dust, and streambed and lake sediment were collected from the Lake Como watershed in Fort Worth, Texas. Characteristics of CM particles determined by organic petrography and a significant correlation between PAH concentrations and organic carbon in coal tar, asphalt, and soot indicate that these three CM particle types are the major sources and carriers of PAHs in the watershed. Estimates of the distribution of PAHs in CM particles indicate that coal-tar pitch, used in some pavement sealcoats, is a dominant source of PAHs in the watershed, and contributes as much as 99% of the PAHs in sealed parking lot dust, 92% in unsealed parking lot dust, 88% in commercial area soil, 71% in streambed sediment, and 84% in surficial lake sediment.

Coal-tar-based parking lot sealcoat: an unrecognized source of PAH to settled house dust.

Despite much speculation, the principal factors controlling concentrations of polycyclic aromatic hydrocarbons (PAH) in settled house dust (SHD) have not yet been identified. In response to recent reports that dust from pavement with coal-tar-based sealcoat contains extremely high concentrations of PAH, we measured PAH in SHD from 23 apartments and in dust from their associated parking lots, one-half of which had coal-tar-based sealcoat (CT). The median concentration of total PAH (T-PAH) in dust from CT parking lots (4760 microg/g, n = 11) was 530 times higher than that from parking lots with other pavement surface types (asphalt-based sealcoat, unsealed asphalt, concrete [median 9.0 microg/g, n = 12]). T-PAH in SHD from apartments with CT parking lots (median 129 microg/g) was 25 times higher than that in SHD from apartments with parking lots with other pavement surface types (median 5.1 microg/g). Presence or absence of CT on a parking lot explained 48% of the variance in log-transformed T-PAH in SHD. Urban land-use intensity near the residence also had a significant but weaker relation to T-PAH. No other variables tested, including carpeting, frequency of vacuuming, and indoor burning, were significant.

Enantiomer fractions of chlordane components in sediment from U.S. Geological Survey sites in lakes and rivers.

Spatial, temporal, and sediment-type trends in enantiomer signatures were evaluated for cis- and trans-chlordane (CC, TC) in archived core, suspended, and surficial-sediment samples from six lake, reservoir, and river sites across the United States. The enantiomer fractions (EFs) measured in these samples are in good agreement with those reported for sediment, soil, and air samples in previous studies. The chlordane EFs were generally close to the racemic value of 0.5, with CC values ranging from 0.493 to 0.527 (usually >0.5) and TC values from 0.463 to 0.53 (usually <0.5). EF changes with core depth were detected for TC and CC in some cores, with the most non-racemic values near the top of the core. Surficial and suspended sediments generally have EF values similar to the top core layers but are often more non-racemic, indicating that enantioselective degradation is occurring before soils are eroded and deposited into bottom sediments. We hypothesize that rapid losses (desorption or degradation) from suspended sediments of the more bioavailable chlordane fraction during transport and initial deposition could explain the apparent shift to more racemic EF values in surficial and top core sediments. Near racemic CC and TC in the core profiles suggest minimal alteration of chlordane from biotic degradation, unless it is via non-enantioselective processes. EF values for the heptachlor degradate, heptachlor epoxide (HEPX), determined in surficial sediments from one location only were always non-racemic (EF approximately 0.66), were indicative of substantial biotic processing, and followed reported EF trends.

Fipronil and its degradates in indoor and outdoor dust.

Fipronil is a potent insecticide used for control of termites, fleas, roaches, ants, and other pests. We measured fipronil, fipronil sulfide, and desulfinyl fipronil concentrations in indoor and outdoor dust from 24 residences in Austin, Texas. At least one of these three fipronil compounds was detected in every sample. Fipronil accounted for most of the total fipronil (T-fipronil; fipronil + desulfinyl fipronil + fipronil sulfide), followed by desulfinyl fipronil and fipronil sulfide. Nineteen of 24 samples of indoor dust had T-fipronil concentrations less than 270 microg/kg; the remaining five had concentrations from 1320 to 14,200 microg/kg. All three of the residences with a dog on which a flea-control product containing fipronil was used were among the five residences with elevated fipronil concentrations. In outdoor dust all concentrations of T-fipronil were less than 70 microg/kg with one exception (430 microg/kg). For every residence, the concentration of T-fipronil in indoor dust exceeded that in outdoor dust, and the median concentration of T-fipronil was 15 times higher indoors than outdoors.

PAHs underfoot: contaminated dust from coal-tar sealcoated pavement is widespread in the United States.

We reported in 2005 that runoff from parking lots treated with coal-tar-based sealcoat was a major source of polycyclic aromatic hydrocarbons (PAHs) to streams in Austin, Texas. Here we present new data from nine U.S. cities that show nationwide patterns in concentrations of PAHs associated with sealcoat. Dust was swept from parking lots in six cities in the central and eastern U.S., where coal-tar-based sealcoat dominates use, and three cities in the western U.S., where asphalt-based sealcoat dominates use. For six central and eastern cities, median SigmaPAH concentrations in dust from sealcoated and unsealcoated pavement are 2200 and 27 mg/kg, respectively. For three western cities, median SigmaPAH concentrations in dust from sealcoated and unsealcoated pavement are similar and very low (2.1 and 0.8 mg/kg, respectively). Lakes in the central and eastern cities where pavement was sampled have bottom sediments with higher PAH concentrations than do those in the western cities relative to degree of urbanization. Bottom-sediment PAH assemblages are similar to those of sealcoated pavement dust regionally, implicating coal-tar-based sealcoat as a PAH source to the central and eastern lakes. Concentrations of benzo[a]pyrene in dustfrom coal-tarsealcoated pavement and adjacent soils greatly exceed generic soil screening levels, suggesting that research on human-health risk is warranted.

Effects of Hurricanes Katrina and Rita on the chemistry of bottom sediments in Lake Pontchartrain, Louisiana, U.S.A.

The effects of Hurricanes Katrina and Rita and the subsequent unwatering of New Orleans, Louisiana, on the sediment chemistry of Lake Pontchartrain were evaluated by chemical analysis of samples of street mud and suspended and bottom sediments. The highest concentrations of urban-related elements and compounds (e.g., Pb, Zn, polycyclic aromatic hydrocarbons, and chlordane) in bottom sediments exceeded median concentrations in U.S. urban lakes and sediment-quality guidelines. The extent of the elevated concentrations was limited, however, to within a few hundred meters of the mouth of the 17th Street Canal, similar to results of historical assessments. Chemical and radionuclide analysis of pre- and post-Hurricane Rita samples indicates that remobilization of near-shore sediment by lake currents and storms is an ongoing process. The effects of Hurricanes Katrina and Rita on the sediment chemistry of Lake Pontchartrain are limited spatially and are most likely transitory.

Parking lot sealcoat: an unrecognized source of urban polycyclic aromatic hydrocarbons.

Polycyclic aromatic hydrocarbons (PAHs) are a ubiquitous contaminant in urban environments. Although numerous sources of PAHs to urban runoff have been identified, their relative importance remains uncertain. We show that a previously unidentified source of urban PAHs, parking lot sealcoat, may dominate loading of PAHs to urban water bodies in the United States. Particles in runoff from parking lots with coal-tar emulsion sealcoat had mean concentrations of PAHs of 3500 mg/kg, 65 times higher than the mean concentration from unsealed asphalt and cement lots. Diagnostic ratios of individual PAHs indicating sources are similar for particles from coal-tar emulsion sealed lots and suspended sediment from four urban streams. Contaminant yields projected to the watershed scale for the four associated watersheds indicate that runoff from sealed parking lots could account for the majority of stream PAH loads.