Drew Luellen - Academia.edu (original) (raw)
Papers by Drew Luellen
Environment International
Environmental Science and Pollution Research
Environmental Science Technology, Feb 21, 2012
Polybrominated diphenyl ethers (PBDEs) have been used extensively to flame-retard polymers and te... more Polybrominated diphenyl ethers (PBDEs) have been used extensively to flame-retard polymers and textiles. These persistent chemicals enter wastewater streams following manufacture, use, and disposal, concentrating in the settled solids during treatment. Land application of stabilized sewage sludge (known as biosolids) can contribute PBDEs to terrestrial systems. Monitoring sludge/biosolids contaminant burdens may be valuable in revealing trends in societal chemical usage and environmental release. In archived Chicago area sludges/biosolids from 1975 to 2008, penta-BDE concentrations increased and then plateaued after about 2000. Penta-BDE manufacture in the United States ended in December 2004. Deca-BDE concentrations in biosolids rose from 1995 to 2008, doubling on a 5-year interval. Evaluation of U.S. Environmental Protection Agency Targeted National Sewage Sludge Survey data from 2006 to 2007 revealed highest penta-BDE biosolids levels from western and lowest from northeastern wastewater treatment plants (2120 and 1530 μg/kg, respectively), consistent with patterns reported in some recent indoor dust and human blood studies. No significant regional trends were observed for deca-BDE concentrations. Congener patterns in contemporary Chicago biosolids support the contention that BDE-209 can be dehalogenated to less brominated congeners. Biosolids application on agricultural fields increased PBDE soil concentrations. However, corn grown thereon did not exhibit measurable PBDE uptake; perhaps due to low bioavailability of the biosolids-associated flame retardants.
ABSTRACT Background: Deca-BDE, a polybrominated diphenyl ether (PBDE)-based flame retardant , is ... more ABSTRACT Background: Deca-BDE, a polybrominated diphenyl ether (PBDE)-based flame retardant , is persistent, widespread in the environment, and abundant in treated sewage sludge (TSS) from some wastewater treatment plants. We evaluated whether concentrations of the primary component congener of deca-BDE, BDE-209, in pine and cedar needle samples were related to proximity to sludge land-application sites. Methods: We collected pine and eastern cedar needles within 1.5 km of sites where TSS from municipalities A&B was land-applied and comparison areas more than 8 km from application sites. We determined concentrations of BDE-209 using GC/MS. Linear regression was used to evaluate relationships between concentrations of BDE-209 and proximity to houses, businesses, and quantities of TSS applied considering weather conditions during and following application. Results: BDE-209 concentrations in TSS grab samples were three orders of magnitude higher in municipality A than B. Mean BDE-209 concentrations in needle samples were 7.32 ng/g near sludge application sites and 7.58 in comparison areas. In areas near municipality B application, BDE-209 concentrations were related to the number of buildings within 100 m (R2=0.11) but not to sludge application. Near municipality A application sites, BDE-209 concentrations were not related to the numbers of buildings but were elevated within 1.2 km of TSS application sites, considering the percent solids, application quantities, and weather conditions (R2=0.13). Conclusions: Concentrations of Deca-BDE were elevated in pine needles samples near sites where TSS with high source concentrations was land-applied. This provides direct evidence that chemical contaminants from TSS land application can migrate into neighboring communities.
Background: Deca-BDE, a polybrominated diphenyl ether (PBDE)-based flame retardant , is persisten... more Background: Deca-BDE, a polybrominated diphenyl ether (PBDE)-based flame retardant , is persistent, widespread in the environment, and abundant in treated sewage sludge (TSS) from some wastewater treatment plants. We evaluated whether concentrations of the primary component congener of deca-BDE, BDE-209, in pine and cedar needle samples were related to proximity to sludge land-application sites. Methods: We collected pine and eastern cedar needles within 1.5 km of sites where TSS from municipalities A&B was land-applied and comparison areas more than 8 km from application sites. We determined concentrations of BDE-209 using GC/MS. Linear regression was used to evaluate relationships between concentrations of BDE-209 and proximity to houses, businesses, and quantities of TSS applied considering weather conditions during and following application. Results: BDE-209 concentrations in TSS grab samples were three orders of magnitude higher in municipality A than B. Mean BDE-209 concentrat...
Environmental Science & Technology, 2011
Polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecane (HBCD) are common flame retarda... more Polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecane (HBCD) are common flame retardants in polymers and textiles. Recognition of the persistent, bioaccumulative, and toxic properties of PBDEs has prompted reductions in their use. In contrast, HBCD has received less scrutiny. The U.S has historically been a dominant BFR consumer. However, the few publications on HBCD in wildlife here suggest modest levels compared to Asian and European studies. In contrast, the HBCD concentrations we detected in U.S. fish are among the highest reported in the world. The temporal trends observed suggest that HBCD use may have risen, and that of Penta-BDE declined, following the 2004 termination of its U.S. manufacture. For example, Hyco River carp collected in 1999-2002 exhibited a mean ∑HBCD (sum of α-, β- and γ-HBCD) concentration of only 13 ng/g (lipid weight basis), but was 4640 ng/g in fish collected in 2006-2007. In contrast, the mean ∑PBDE level in these same fish decreased from 40,700 ng/g in 1999-2002 to 9140 ng/g in 2006-2007. Concentrations of HBCD and PBDEs in several Hyco River fish species exceeded those from rivers less influenced by manufacturing outfalls. Results support the contention that textile-related production, relative to its BFR market share, may release disproportionately large amounts of HBCD to the environment.
Environmental Science & Technology, 2012
Polybrominated diphenyl ethers (PBDEs) have been used extensively to flame-retard polymers and te... more Polybrominated diphenyl ethers (PBDEs) have been used extensively to flame-retard polymers and textiles. These persistent chemicals enter wastewater streams following manufacture, use, and disposal, concentrating in the settled solids during treatment. Land application of stabilized sewage sludge (known as biosolids) can contribute PBDEs to terrestrial systems. Monitoring sludge/biosolids contaminant burdens may be valuable in revealing trends in societal chemical usage and environmental release. In archived Chicago area sludges/biosolids from 1975 to 2008, penta-BDE concentrations increased and then plateaued after about 2000. Penta-BDE manufacture in the United States ended in December 2004. Deca-BDE concentrations in biosolids rose from 1995 to 2008, doubling on a 5-year interval. Evaluation of U.S. Environmental Protection Agency Targeted National Sewage Sludge Survey data from 2006 to 2007 revealed highest penta-BDE biosolids levels from western and lowest from northeastern wastewater treatment plants (2120 and 1530 μg/kg, respectively), consistent with patterns reported in some recent indoor dust and human blood studies. No significant regional trends were observed for deca-BDE concentrations. Congener patterns in contemporary Chicago biosolids support the contention that BDE-209 can be dehalogenated to less brominated congeners. Biosolids application on agricultural fields increased PBDE soil concentrations. However, corn grown thereon did not exhibit measurable PBDE uptake; perhaps due to low bioavailability of the biosolids-associated flame retardants.
Environmental Science Technology, Oct 1, 2011
Polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecane (HBCD) are common flame retarda... more Polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecane (HBCD) are common flame retardants in polymers and textiles. Recognition of the persistent, bioaccumulative, and toxic properties of PBDEs has prompted reductions in their use. In contrast, HBCD has received less scrutiny. The U.S has historically been a dominant BFR consumer. However, the few publications on HBCD in wildlife here suggest modest levels compared to Asian and European studies. In contrast, the HBCD concentrations we detected in U.S. fish are among the highest reported in the world. The temporal trends observed suggest that HBCD use may have risen, and that of Penta-BDE declined, following the 2004 termination of its U.S. manufacture. For example, Hyco River carp collected in 1999-2002 exhibited a mean ∑HBCD (sum of α-, β- and γ-HBCD) concentration of only 13 ng/g (lipid weight basis), but was 4640 ng/g in fish collected in 2006-2007. In contrast, the mean ∑PBDE level in these same fish decreased from 40,700 ng/g in 1999-2002 to 9140 ng/g in 2006-2007. Concentrations of HBCD and PBDEs in several Hyco River fish species exceeded those from rivers less influenced by manufacturing outfalls. Results support the contention that textile-related production, relative to its BFR market share, may release disproportionately large amounts of HBCD to the environment.
Environmental pollution (Barking, Essex : 1987), Jan 24, 2015
Historical persistent organic pollutants (POPs) are banned from Antarctica under international tr... more Historical persistent organic pollutants (POPs) are banned from Antarctica under international treaty; but contemporary-use POPs can enter as additives within polymer and textile products. Over their useful lives these products may release additives in-situ. Indeed, we observed 226 and 109 ng/g dry weight (dw) of the total concentrations of α-, β- and γ-hexabromocyclododecane (HBCD) in indoor dust from McMurdo Station (U.S.) and Scott Station (New Zealand), respectively. Sewage sludge collected from wastewater treatment facilities at these stations exhibited ∑HBCD of 45 and 69 ng/g dw, respectively. Contaminants originally within the bases may exit to the local outdoor environment via wastewaters. Near McMurdo, maximum ∑HBCD levels in surficial marine sediments and aquatic biota (invertebrates and fish) were 2350 ng/g (total organic carbon basis) and 554 ng/g lipid weight, respectively. Levels declined with distance from McMurdo. Our results illustrate that Antarctic research statio...
Science of The Total Environment, 2006
In late 1975, it was discovered that a manufacturing facility had not only exposed workers to the... more In late 1975, it was discovered that a manufacturing facility had not only exposed workers to the chlorinated pesticide, Kepone, but had also severely contaminated the James River estuary. To assess the potential for the public to be exposed to Kepone through the consumption of contaminated seafood, the Commonwealth of Virginia initiated a finfish-monitoring program in late 1975. Over 13,000 samples have been collected and analyzed as part of this effort. Kepone levels in most species began falling when the production of Kepone ended, but the average concentrations remained over the action limit of 0.3 microg g(-1) wet weight until the early 1980s. By 1988 few fish contained Kepone concentrations greater than the action limit. Kepone is still detected in the majority of white perch and striped bass samples taken from the James River and a fish consumption advisory is still in effect thirty years after the source of contamination was removed.
Environmental Science & Technology, 2012
Polybrominated diphenyl ethers (PBDEs) have been used extensively to flame-retard polymers and te... more Polybrominated diphenyl ethers (PBDEs) have been used extensively to flame-retard polymers and textiles. These persistent chemicals enter wastewater streams following manufacture, use, and disposal, concentrating in the settled solids during treatment. Land application of stabilized sewage sludge (known as biosolids) can contribute PBDEs to terrestrial systems. Monitoring sludge/biosolids contaminant burdens may be valuable in revealing trends in societal chemical usage and environmental release. In archived Chicago area sludges/biosolids from 1975 to 2008, penta-BDE concentrations increased and then plateaued after about 2000. Penta-BDE manufacture in the United States ended in December 2004. Deca-BDE concentrations in biosolids rose from 1995 to 2008, doubling on a 5-year interval. Evaluation of U.S. Environmental Protection Agency Targeted National Sewage Sludge Survey data from 2006 to 2007 revealed highest penta-BDE biosolids levels from western and lowest from northeastern wastewater treatment plants (2120 and 1530 μg/kg, respectively), consistent with patterns reported in some recent indoor dust and human blood studies. No significant regional trends were observed for deca-BDE concentrations. Congener patterns in contemporary Chicago biosolids support the contention that BDE-209 can be dehalogenated to less brominated congeners. Biosolids application on agricultural fields increased PBDE soil concentrations. However, corn grown thereon did not exhibit measurable PBDE uptake; perhaps due to low bioavailability of the biosolids-associated flame retardants.
Environmental Science & Technology, 2002
The use of semipermeable membrane devices (SPMDs) has become common in environmental sampling of ... more The use of semipermeable membrane devices (SPMDs) has become common in environmental sampling of nonpolar organic contaminants, yet few data exist for the uptake or sampling rates of polycyclic aromatic hydrocarbons (PAH). Two separate laboratory calibration experiments were conducted to determine the sampling rates of 28 individual PAH and 19 homologues. PAH with a log K ow > 4.5 remained in the linear uptake phase for 30 days, but PAH with a log K ow < 4.5 began to approach steady state within 15 days. Sampling rates, corrected for dissolved organic carbon, ranged from 2.11 to 6.06 L d -1 . Shear flow across the membrane had no statistically significant effect on rates over the range of 0.01-0.50 cm s -1 . Field verification of these sampling rates yielded agreement within about a factor of 2 for most PAH and a factor of 4 for all PAH. The worst agreement was for the most hydrophobic PAH, where partitioning into dissolved and particulate organic carbon pools are more important and less certain. These SPMD sampling rate data will allow quantitative estimations of freely dissolved concentrations of 47 compounds that are commonly used for PAH and petroleum product source identification and allocation.
Chemosphere, 2003
Semipermeable membrane devices (SPMDs) are commonly used as a time-integrated measure of aqueous ... more Semipermeable membrane devices (SPMDs) are commonly used as a time-integrated measure of aqueous concentrations of persistent hydrophobic chemicals, including PAH, pesticides, dioxins, and PCBs. Another class of persistent hydrophobic chemicals is petroleum biomarker compounds (hopanes and steranes) that are used for hydrocarbon source identification and allocation. In this study three different passive sampling device designs were exposed to a complex hydrocarbon mixture (Alaska North Slope crude) in a laboratory experiment to determine uptake rates of biomarkers into SPMDs. In addition to the standard triolein filled SPMDs, iso-octane filled SPMDs (ISPMDs) and unfilled low-density polyethylene strips (PESDs) were tested. Uptake rates and effective sampling rates were determined for 53 compounds. There was little variation in sampling rates among the individual biomarkers; average values (l d À1 ) for hopanes were 0.43 AE 0.07 (PESD), 0.33 AE 0.06 (SPMD), and 0.44 AE 0.03 (ISPMD) and average sterane sampling rates were 0.57 AE 0.04 (PESD), 0.42 AE 0.03 (SPMD), and 0.53 AE 0.03 (ISPMD). The primary reason for biomarker analysis is for source discrimination of petroleum. Nineteen different diagnostic ratios were measured, and were found to be remarkably well conserved between the oil, water, and all three devices. This indicates that SPMDs, PESDs, and ISPMDs should each be effective for source discrimination studies of petroleum contamination.
Environmental Science & Technology, 2011
Environment International
Environmental Science and Pollution Research
Environmental Science Technology, Feb 21, 2012
Polybrominated diphenyl ethers (PBDEs) have been used extensively to flame-retard polymers and te... more Polybrominated diphenyl ethers (PBDEs) have been used extensively to flame-retard polymers and textiles. These persistent chemicals enter wastewater streams following manufacture, use, and disposal, concentrating in the settled solids during treatment. Land application of stabilized sewage sludge (known as biosolids) can contribute PBDEs to terrestrial systems. Monitoring sludge/biosolids contaminant burdens may be valuable in revealing trends in societal chemical usage and environmental release. In archived Chicago area sludges/biosolids from 1975 to 2008, penta-BDE concentrations increased and then plateaued after about 2000. Penta-BDE manufacture in the United States ended in December 2004. Deca-BDE concentrations in biosolids rose from 1995 to 2008, doubling on a 5-year interval. Evaluation of U.S. Environmental Protection Agency Targeted National Sewage Sludge Survey data from 2006 to 2007 revealed highest penta-BDE biosolids levels from western and lowest from northeastern wastewater treatment plants (2120 and 1530 μg/kg, respectively), consistent with patterns reported in some recent indoor dust and human blood studies. No significant regional trends were observed for deca-BDE concentrations. Congener patterns in contemporary Chicago biosolids support the contention that BDE-209 can be dehalogenated to less brominated congeners. Biosolids application on agricultural fields increased PBDE soil concentrations. However, corn grown thereon did not exhibit measurable PBDE uptake; perhaps due to low bioavailability of the biosolids-associated flame retardants.
ABSTRACT Background: Deca-BDE, a polybrominated diphenyl ether (PBDE)-based flame retardant , is ... more ABSTRACT Background: Deca-BDE, a polybrominated diphenyl ether (PBDE)-based flame retardant , is persistent, widespread in the environment, and abundant in treated sewage sludge (TSS) from some wastewater treatment plants. We evaluated whether concentrations of the primary component congener of deca-BDE, BDE-209, in pine and cedar needle samples were related to proximity to sludge land-application sites. Methods: We collected pine and eastern cedar needles within 1.5 km of sites where TSS from municipalities A&B was land-applied and comparison areas more than 8 km from application sites. We determined concentrations of BDE-209 using GC/MS. Linear regression was used to evaluate relationships between concentrations of BDE-209 and proximity to houses, businesses, and quantities of TSS applied considering weather conditions during and following application. Results: BDE-209 concentrations in TSS grab samples were three orders of magnitude higher in municipality A than B. Mean BDE-209 concentrations in needle samples were 7.32 ng/g near sludge application sites and 7.58 in comparison areas. In areas near municipality B application, BDE-209 concentrations were related to the number of buildings within 100 m (R2=0.11) but not to sludge application. Near municipality A application sites, BDE-209 concentrations were not related to the numbers of buildings but were elevated within 1.2 km of TSS application sites, considering the percent solids, application quantities, and weather conditions (R2=0.13). Conclusions: Concentrations of Deca-BDE were elevated in pine needles samples near sites where TSS with high source concentrations was land-applied. This provides direct evidence that chemical contaminants from TSS land application can migrate into neighboring communities.
Background: Deca-BDE, a polybrominated diphenyl ether (PBDE)-based flame retardant , is persisten... more Background: Deca-BDE, a polybrominated diphenyl ether (PBDE)-based flame retardant , is persistent, widespread in the environment, and abundant in treated sewage sludge (TSS) from some wastewater treatment plants. We evaluated whether concentrations of the primary component congener of deca-BDE, BDE-209, in pine and cedar needle samples were related to proximity to sludge land-application sites. Methods: We collected pine and eastern cedar needles within 1.5 km of sites where TSS from municipalities A&B was land-applied and comparison areas more than 8 km from application sites. We determined concentrations of BDE-209 using GC/MS. Linear regression was used to evaluate relationships between concentrations of BDE-209 and proximity to houses, businesses, and quantities of TSS applied considering weather conditions during and following application. Results: BDE-209 concentrations in TSS grab samples were three orders of magnitude higher in municipality A than B. Mean BDE-209 concentrat...
Environmental Science & Technology, 2011
Polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecane (HBCD) are common flame retarda... more Polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecane (HBCD) are common flame retardants in polymers and textiles. Recognition of the persistent, bioaccumulative, and toxic properties of PBDEs has prompted reductions in their use. In contrast, HBCD has received less scrutiny. The U.S has historically been a dominant BFR consumer. However, the few publications on HBCD in wildlife here suggest modest levels compared to Asian and European studies. In contrast, the HBCD concentrations we detected in U.S. fish are among the highest reported in the world. The temporal trends observed suggest that HBCD use may have risen, and that of Penta-BDE declined, following the 2004 termination of its U.S. manufacture. For example, Hyco River carp collected in 1999-2002 exhibited a mean ∑HBCD (sum of α-, β- and γ-HBCD) concentration of only 13 ng/g (lipid weight basis), but was 4640 ng/g in fish collected in 2006-2007. In contrast, the mean ∑PBDE level in these same fish decreased from 40,700 ng/g in 1999-2002 to 9140 ng/g in 2006-2007. Concentrations of HBCD and PBDEs in several Hyco River fish species exceeded those from rivers less influenced by manufacturing outfalls. Results support the contention that textile-related production, relative to its BFR market share, may release disproportionately large amounts of HBCD to the environment.
Environmental Science & Technology, 2012
Polybrominated diphenyl ethers (PBDEs) have been used extensively to flame-retard polymers and te... more Polybrominated diphenyl ethers (PBDEs) have been used extensively to flame-retard polymers and textiles. These persistent chemicals enter wastewater streams following manufacture, use, and disposal, concentrating in the settled solids during treatment. Land application of stabilized sewage sludge (known as biosolids) can contribute PBDEs to terrestrial systems. Monitoring sludge/biosolids contaminant burdens may be valuable in revealing trends in societal chemical usage and environmental release. In archived Chicago area sludges/biosolids from 1975 to 2008, penta-BDE concentrations increased and then plateaued after about 2000. Penta-BDE manufacture in the United States ended in December 2004. Deca-BDE concentrations in biosolids rose from 1995 to 2008, doubling on a 5-year interval. Evaluation of U.S. Environmental Protection Agency Targeted National Sewage Sludge Survey data from 2006 to 2007 revealed highest penta-BDE biosolids levels from western and lowest from northeastern wastewater treatment plants (2120 and 1530 μg/kg, respectively), consistent with patterns reported in some recent indoor dust and human blood studies. No significant regional trends were observed for deca-BDE concentrations. Congener patterns in contemporary Chicago biosolids support the contention that BDE-209 can be dehalogenated to less brominated congeners. Biosolids application on agricultural fields increased PBDE soil concentrations. However, corn grown thereon did not exhibit measurable PBDE uptake; perhaps due to low bioavailability of the biosolids-associated flame retardants.
Environmental Science Technology, Oct 1, 2011
Polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecane (HBCD) are common flame retarda... more Polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecane (HBCD) are common flame retardants in polymers and textiles. Recognition of the persistent, bioaccumulative, and toxic properties of PBDEs has prompted reductions in their use. In contrast, HBCD has received less scrutiny. The U.S has historically been a dominant BFR consumer. However, the few publications on HBCD in wildlife here suggest modest levels compared to Asian and European studies. In contrast, the HBCD concentrations we detected in U.S. fish are among the highest reported in the world. The temporal trends observed suggest that HBCD use may have risen, and that of Penta-BDE declined, following the 2004 termination of its U.S. manufacture. For example, Hyco River carp collected in 1999-2002 exhibited a mean ∑HBCD (sum of α-, β- and γ-HBCD) concentration of only 13 ng/g (lipid weight basis), but was 4640 ng/g in fish collected in 2006-2007. In contrast, the mean ∑PBDE level in these same fish decreased from 40,700 ng/g in 1999-2002 to 9140 ng/g in 2006-2007. Concentrations of HBCD and PBDEs in several Hyco River fish species exceeded those from rivers less influenced by manufacturing outfalls. Results support the contention that textile-related production, relative to its BFR market share, may release disproportionately large amounts of HBCD to the environment.
Environmental pollution (Barking, Essex : 1987), Jan 24, 2015
Historical persistent organic pollutants (POPs) are banned from Antarctica under international tr... more Historical persistent organic pollutants (POPs) are banned from Antarctica under international treaty; but contemporary-use POPs can enter as additives within polymer and textile products. Over their useful lives these products may release additives in-situ. Indeed, we observed 226 and 109 ng/g dry weight (dw) of the total concentrations of α-, β- and γ-hexabromocyclododecane (HBCD) in indoor dust from McMurdo Station (U.S.) and Scott Station (New Zealand), respectively. Sewage sludge collected from wastewater treatment facilities at these stations exhibited ∑HBCD of 45 and 69 ng/g dw, respectively. Contaminants originally within the bases may exit to the local outdoor environment via wastewaters. Near McMurdo, maximum ∑HBCD levels in surficial marine sediments and aquatic biota (invertebrates and fish) were 2350 ng/g (total organic carbon basis) and 554 ng/g lipid weight, respectively. Levels declined with distance from McMurdo. Our results illustrate that Antarctic research statio...
Science of The Total Environment, 2006
In late 1975, it was discovered that a manufacturing facility had not only exposed workers to the... more In late 1975, it was discovered that a manufacturing facility had not only exposed workers to the chlorinated pesticide, Kepone, but had also severely contaminated the James River estuary. To assess the potential for the public to be exposed to Kepone through the consumption of contaminated seafood, the Commonwealth of Virginia initiated a finfish-monitoring program in late 1975. Over 13,000 samples have been collected and analyzed as part of this effort. Kepone levels in most species began falling when the production of Kepone ended, but the average concentrations remained over the action limit of 0.3 microg g(-1) wet weight until the early 1980s. By 1988 few fish contained Kepone concentrations greater than the action limit. Kepone is still detected in the majority of white perch and striped bass samples taken from the James River and a fish consumption advisory is still in effect thirty years after the source of contamination was removed.
Environmental Science & Technology, 2012
Polybrominated diphenyl ethers (PBDEs) have been used extensively to flame-retard polymers and te... more Polybrominated diphenyl ethers (PBDEs) have been used extensively to flame-retard polymers and textiles. These persistent chemicals enter wastewater streams following manufacture, use, and disposal, concentrating in the settled solids during treatment. Land application of stabilized sewage sludge (known as biosolids) can contribute PBDEs to terrestrial systems. Monitoring sludge/biosolids contaminant burdens may be valuable in revealing trends in societal chemical usage and environmental release. In archived Chicago area sludges/biosolids from 1975 to 2008, penta-BDE concentrations increased and then plateaued after about 2000. Penta-BDE manufacture in the United States ended in December 2004. Deca-BDE concentrations in biosolids rose from 1995 to 2008, doubling on a 5-year interval. Evaluation of U.S. Environmental Protection Agency Targeted National Sewage Sludge Survey data from 2006 to 2007 revealed highest penta-BDE biosolids levels from western and lowest from northeastern wastewater treatment plants (2120 and 1530 μg/kg, respectively), consistent with patterns reported in some recent indoor dust and human blood studies. No significant regional trends were observed for deca-BDE concentrations. Congener patterns in contemporary Chicago biosolids support the contention that BDE-209 can be dehalogenated to less brominated congeners. Biosolids application on agricultural fields increased PBDE soil concentrations. However, corn grown thereon did not exhibit measurable PBDE uptake; perhaps due to low bioavailability of the biosolids-associated flame retardants.
Environmental Science & Technology, 2002
The use of semipermeable membrane devices (SPMDs) has become common in environmental sampling of ... more The use of semipermeable membrane devices (SPMDs) has become common in environmental sampling of nonpolar organic contaminants, yet few data exist for the uptake or sampling rates of polycyclic aromatic hydrocarbons (PAH). Two separate laboratory calibration experiments were conducted to determine the sampling rates of 28 individual PAH and 19 homologues. PAH with a log K ow > 4.5 remained in the linear uptake phase for 30 days, but PAH with a log K ow < 4.5 began to approach steady state within 15 days. Sampling rates, corrected for dissolved organic carbon, ranged from 2.11 to 6.06 L d -1 . Shear flow across the membrane had no statistically significant effect on rates over the range of 0.01-0.50 cm s -1 . Field verification of these sampling rates yielded agreement within about a factor of 2 for most PAH and a factor of 4 for all PAH. The worst agreement was for the most hydrophobic PAH, where partitioning into dissolved and particulate organic carbon pools are more important and less certain. These SPMD sampling rate data will allow quantitative estimations of freely dissolved concentrations of 47 compounds that are commonly used for PAH and petroleum product source identification and allocation.
Chemosphere, 2003
Semipermeable membrane devices (SPMDs) are commonly used as a time-integrated measure of aqueous ... more Semipermeable membrane devices (SPMDs) are commonly used as a time-integrated measure of aqueous concentrations of persistent hydrophobic chemicals, including PAH, pesticides, dioxins, and PCBs. Another class of persistent hydrophobic chemicals is petroleum biomarker compounds (hopanes and steranes) that are used for hydrocarbon source identification and allocation. In this study three different passive sampling device designs were exposed to a complex hydrocarbon mixture (Alaska North Slope crude) in a laboratory experiment to determine uptake rates of biomarkers into SPMDs. In addition to the standard triolein filled SPMDs, iso-octane filled SPMDs (ISPMDs) and unfilled low-density polyethylene strips (PESDs) were tested. Uptake rates and effective sampling rates were determined for 53 compounds. There was little variation in sampling rates among the individual biomarkers; average values (l d À1 ) for hopanes were 0.43 AE 0.07 (PESD), 0.33 AE 0.06 (SPMD), and 0.44 AE 0.03 (ISPMD) and average sterane sampling rates were 0.57 AE 0.04 (PESD), 0.42 AE 0.03 (SPMD), and 0.53 AE 0.03 (ISPMD). The primary reason for biomarker analysis is for source discrimination of petroleum. Nineteen different diagnostic ratios were measured, and were found to be remarkably well conserved between the oil, water, and all three devices. This indicates that SPMDs, PESDs, and ISPMDs should each be effective for source discrimination studies of petroleum contamination.
Environmental Science & Technology, 2011