NJ Department of Health
Community Exposure to Perfluoroalkyl and Polyfluoroalkyl Substances (PFASs), an Emerging
Public Health IssueChang Ho Yu, Ph.D.Research Scientist
Environmental and Chemical Laboratory Services (ECLS), NJDOH-PHEL
June 14, 20172017 APHL Annual Meeting & Eleventh Government Environmental Laboratory Conference at
Rhode Island Convention Center, Providence, Rhode Island
NJ Department of Health
Contents What are PFASs?
o Physicochemical propertieso Classifications and major typeso Manufacturing processeso Common useso Timeline for PFASs production, analysis, and regulation
Why PFASs are challenges to public health?o Proximity (sources)o Exposure pathwayso Persistence (biological behaviors) o Toxicityo Analytical perspectives
How to address PFASs issues?o CDC’s national biomonitoring programo Other states’ biomonitoring programs
NJDOH responses to emerging contaminants, PFASso Method development/optimizationo NJ biomonitoring (BM) projects
• Project I (general NJ residents)• Project II (local communities)• Project III (pregnant women)
o Challenges & future research directions
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Part I: What are PFASs?
PFASs: Man-made chemicals by replacing fluorine (F) atom(s) into hydrogen (H) in organic compounds
Cn:F2n±1
o chemically/thermally stableo hydrophobic & lipophobico slippery propertieso persistent in environment
Applicationso non-sticking cook-wares, food containers,
consumer products; o water-proof clothing;o stain resistant coating;o fire-fighting foams; ando surfactant/emulsifier for industrial uses.
C8HF15O2
C8HF17O3S
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Perfluoroalkyl & Polyfluoroalkyl
Substances (PFASs)
Perfluoroalkyl Substances
Polyfluoroalkyl Substances
Perfluoroalkane Sulfonamides
(FASAs)
Perfluoroalkyl Acids (PFAAs)
Perfluoroalkane Sulfonamido Substances Perfluoroalkane
Sulfonamidoethanols (FASEs)
Fluorotelomer Substances
PerfluoroalkaneSulfonamidoacetic
Acids (FASAAs)
Fluorotelomer Alcohols (FTOHs)
Polyfluoroalkyl Phosphoric Acid
Esters (PAPs)
Perfluoroalkyl Carboxylic Acids
(PFCAs)
Perfluoroalkyl Sulfonic Acids (PFSAs)
PFASs: How Categorized and Named?
Fully Fluorinated
Partially Fluorinated
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Group Target Compounds Chemical Formula
C4 Perfluorobutanesulfonic acid (PFBuS or PFBS) Perfluorobutanoic acid (PFBuA)
C4HF7O2C4HF9O3S
C5 Perfluoropentanoic acid (PFPeA) C5HF9O2
C6 Perfluorohexanesulfonic acid (PFHxS) Perfluorohexanoic acid (PFHxA)
C6HF13O3SC6HF11O2
C7 Perfluoroheptanoic acid (PFHpA) C7HF13O2
C8Perfluorooctanesulfonic acid (PFOS) Perfluorooctanoic acid (PFOA)Perfluorooctanesulfonamide (PFOSA)
C8HF17O3SC8HF15O2C8H2F17NO2S
C9 Perfluorononanoic acid (PFNA) C9HF17O2
C10 Perfluorodecanoic acid (PFDeA or PFDA) C10HF19O2
C11 Perfluoroundecanoic acid (PFUA or PFUnA) 2-(N-methyl-Perfluorooctanesulfonamidoacetic acid (Me-PFOSA-AcOH or NMeFOSAA)
C11HF21O2C11H6F17NO4S
C12 Perfluorododecanoic acid (PFDoA) 2-(N-ethyl-Perfluorooctanesulfonamidoacetic acid (Et-PFOSA-AcOH or NEtFOSAA)
C12HF23O2C12H8F17NO4S
C13 Perfluorotridecanoic acid (PFTrDA) C13HF25O2
C14 Perfluorotetradecanoic acid (PFTA) C14HF27O2
CDC/EPA
CDC
EPA
Long-chain(≥C8)
Short-chain(C4-C6)
Carbon Groups
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Electrochemical fluorination (ECF):o Mixture of branched (~30% in PFOS &
20% in PFOA) and linear (~70% & 80%, respectively) isomers and by-products
o Manufactured @3Mo “Historical” process and phased-out
since 2002 in US; but still used overseas and for PFBuS in US
Telomerization:o Synthetic process by adding free radicals
and resulting in isomerically pure linear products
o Started/Manufactured @DuPonto “Modern” process and still widely usedo Voluntarily switched to shorter chain
compounds (C4-C6)
Manufacturing Techniques
C8H17SO2F + 34HF →
C8F17SO2F + 17H2 →
C8F17SO3H or C8F17SO2X
F(CF2)2I → F(CF2)nI →
F(CF2)nCH2CH2I →
F(CF2)nCH2CH2OH
OSF
POSF
PFOS POSF derivatives
n:2 FTOH
n:2 FTI (Telomer B)
PFEI PFAI (Telomer A)
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Everywhere, around you
Water-proof (Gore-Tex®)
Fast food wrapper
Pop corn bag
Pizza box Nail polish
Stain-proof (Scotchgard®)
Ski wax
Non-sticking cookware
Shampoo
Cleaning products
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Aqueous film forming foam (AFFF) fire-fighting agents
Engineering coatings
Medical devicesTextile, upholstery, and carpet
Oil production
Packaging
Plastics and rubber
Industrial Uses
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Milestone for PFASs – Production, Analysis, and RegulationTime What Happened
1950s 3M: Manufactured PFOSDuPont: Manufactured Teflon®
1969 DOD: AFFF patented as fire fighting foams and implemented throughout the military bases
1980-90s LC-MS/MS developed with detecting ppm to ppb levels
2002 EPA: Initiated voluntary phase-out of PFOS
2005 DuPont: $234 M class action lawsuit in the Ohio river
2000s LC-MS/MS improved to detecting ppt and ppq levels
2006 EPA: Announced PFOA Stewardship Program by reducing 95% in 2010 and 100% in 2015
2009 EPA: Published Method 537 for water
2011 EPA: Published Draft Method for sewage/sludge/biosolids
2012 EPA: UCMR3 signed
2016 EPA: Released health limits for combined PFOS and PFOA not exceeding 70 ppt (ng/L)
2016 NJ: Approved PFNA Maximum Contaminant Level (MCL) of 13 ppt(ng/L) in drinking water
2017 NJ: Recommended PFOA MCL of 14 ppt (ng/L) in drinking water
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Part II: Why Concerns for PFASs?
1. Persistence in the environment
2. Widespread exposure to humans
3. Observed toxicity in animals
4. Insufficient information to
assess human risks
PFASs are matters in terms of:
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How PFASs Travel?
The PFASs release, transport, and exposure pathways to humans. (Oliaei et al., 2013)
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PFAS-contaminated Drinking Water Occurred across US
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Data on PFC drinking water contamination are collected under the Unregulated Contaminant Monitoring Rule (UCMR) for suspectedcontaminants for which the EPA has not established health-based standards under the Safe Drinking Water Act. The drinking water data in this map were taken from the October 2015 UCMR 3 data summary. In addition, the map shows 664 fire- or crash-training sites, identified by the Department of Defense, where a PFC-laced fire suppressant known as Aqueous Film-Forming Foam was used, often for decades. Not all of these sites have been tested for PFCs, but it is likely that all of them are contaminated. Data visualization: Moiz Syed. Sources: EPA and Department of Defense.https://theintercept.com/2015/12/16/toxic-firefighting-foam-has-contaminated-u-s-drinking-water-with-pfcs/
AFFFs Contaminate US Drinking Water
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Exposure Pathways
Drinking Water
Non-dietary from House Dust
Dietary from Food
Consumption
Migrated from Household Products
Dermal Contact
Air esp. from Occupational
Exposures
by Direct Exposures
from PFASs
by Indirect Exposure from
Precursors (e.g., FTOHs, PAPs, FASAs,
FASEs)
Ingestion
Inhalation
Absorption
Human Uptake
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How Processed in the Body?
Oral/Dermal/Pulmonary Absorption
Blood (serum
albumin)
LiverKidney
Urine &
Feces
lost
excreted
IN > OUT Bioaccumulation
metabolized
transported
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Takes Long Time to be Eliminated in Human Body
Study Population/Method Half-life (year)PFOS PFOA PFHxS PFNA
Retired workers/Serum measurements (Olsen et al., 2007)
5.4 [2.4-21.7] 3.8 [1.5-9.1] 8.5 [2.2-27.0] No data
Community residents/Serum measurements
*3.8 (MDH, 2013)
2.3 (Bartell et al., 2010)3.3 (Brede et al., 2010)2.9-10.1 (Seals et al., 2011)*4.8 (MDH, 2013)
*5.6 (MDH, 2013) No data
General population/Urinary excretion (**Zhang et al., 2013)
6.2 (YF)27 (M+OF)
2.1 (YF)2.6 (M+OF)
7.7 (YF)35 (M+OF)
2.5 (YF)4.3 (M+OF)
*Estimated from Minnesota Dept. of Health PFC pilot study results (2008-2010; N=193)**Differences are from loss via menstrual bleeding, pregnancy, and lactation in pre-menopausal women.
Half-lives are varied by PFASs, Study Population or Method
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Health Outcomes
Not easily biodegradableo persistent in environments and
bioaccumulative in biota Highly toxic in animal studies
o disrupting normal endocrine activityo reducing immune functiono causing adverse effects on organs (liver,
pancreas, etc.)o causing developmental problems in
rodent offspring exposed in the womb Limited toxicity in human studies
o suggested similar effects on human health; while failed to find conclusive links
PFASs
Obesity
Cancer
High cholesterol
Immuno-deficiency
Hormone disruption
C8 Science Panel• Mid-Ohio valley communities• PFOA (C8)• Large-scale epidemiological study
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Matrixo Biological
• Blood (serum), milk, semen, etc.o Environmental
• Drinking water (DW), house dust, etc.o Foodo Consumer products
Extractiono Solid phase extraction (SPE)
• Off-line (cartridge or 96-well plate)• On-line (automated unit)
o Solvent extraction in sonicator/microwave oveno Direct injection (for DW)
Analysiso LC-MS : Preferred choice
• Separated by reverse phase silica column with polarity• Ionized in (-)ESI and determined by Quadrupole MS(/MS),
Ion Trap MS(/MS), or Time-of-Flight (ToF) HRMS• Corrected by internal standards
o GC-MS• Derivatized and separated by a capillary column• Ionized in EI, CI, or NCI modes and determined by MS
o 19F Nuclear Magnetic Resonance (NMR) Spectroscopy• Structure/purity of organofluorine compounds• Need a pre-concentration/cleanup
AB Sciex QTRAP 6500
Agilent 6545 Q-TOF
Analytical Perspectives
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Part III: CDC’s National Biomonitoring Program
National Health and Nutrition Examination Survey (NHANES)• Since 1999, PFASs in human sera
have been measured and reported • Period: 1999-ongoing• Subjects: ~2000 kids (12-19) + adults
(>20) across US• Detected >99% of PFOS, PFOA,
PFHxS, and PFNA in general US population
• Decreasing trends of PFASs due to phase-out of PFOS and PFOA.
https://www.cdc.gov/biomonitoring/
NJ Department of Health
Other States’ Biomonitoring Programs in California
Asian/Pacific Islander Community Exposures (ACE) Project• Period: 2016-present• Subjects: 100 Chinese adults in SF bay area
Biomonitoring Exposures Study (BEST)• Period: 2011-present• Subjects: 453 adults in Central ValleyCalifornia Teachers Study (CTS)• Period: 2011-present• Subjects: 2,869 female school teachers in CA
Firefighter Occupational Exposures (FOX) Project• Period: 2010-present• Subjects: 101 firefighters in CAMaternal and Infant Environmental Exposure Project (MIEEP)• Period: 2010-present• Subjects: 92 pregnant women-infant in SF
http://biomonitoring.ca.gov/chemicals/perfluorochemicals-pfcs
More Lab Collaboration Studies for Archived Samplese.g., 3Gs, MAMAS,…etc.
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Other States’ Biomonitoring Program in Minnesota
Community Exposure to PFCs in East Metro, MN• Background: public and private
drinking water contaminated with PFCs in 2000s
• Period: 2008-2014• Subjects: 300 East Metro Residents in
MN• Reduced PFCs in drinking water to
below health-based limits. • Observed declining trends of PFCs in
subjects over time.
http://www.health.state.mn.us/divs/hpcd/tracking/biomonitoring/projects/emetro-landing.html
NJ Department of Health
Other States’ Biomonitoring Program in New York
PFOA in Drinking Water in the Village of Hoosick Falls and Petersburg, NY• Background: public and private drinking water contaminated with PFOA in 2014/2015• Subjects: 2,081 participants in Hoosick Falls & ~1,000 from Petersburg• Period: 2016-ongoing• Hoosick Falls results (GM [Mdn]): 23.5 [28.3] ng/mL; n=2,081. • Preliminary results from Petersburg: 11.7 [10.7] ng/mL; n=55.
https://www.health.ny.gov/environmental/investigations/hoosick/
NJ Department of Health
Other States’ Biomonitoring Program in New Hampshire
PFCs Blood Testing Program in NH• Background: In 2014, elevated PFCs
were found in public wells at Pease Tradeport community in Portsmouth, NH, former Pease Air Force Base. Also, elevated PFOA was detected in private wells, in Southern NH.
• Period: 2015-ongoing• Subjects: 1,578 from Pease
communities & 173 from S. NH (to date)
• Pease data shows serum PFCs were higher than general US and lower than other environmentally exposed communities.
https://www.dhhs.nh.gov/dphs/pfcs/blood-testing.htm
NJ Department of Health
Part IV: NJDOH Responses to an Emerging Contaminant, PFASs
Statement:1. NJ has an ongoing contamination
issue in Paulsboro (detected PFASs in public water).
2. Biomonitoring including PFASs greatly helps to preventing potential health outcomes.
The PFASs measured in NJ public water system in 2010-2013. (Source: Post et al., 2013)
NJ BM Project
General Population
Community Residents
Pregnant Women
NJ Department of Health
NJDOH Method
Analysis Column Agilent XDB-C83.0 x 100 mm, 3.5-micron
Aqueous Solution(Mobile Phase A)
10mM Ammonium Acetate in Water (pH=4.3)
Organic Acid (Mobile Phase B)
50% Methanol + 50% Acetonitrile
Gradient Program
1:30 (B:65%) -7:30 (B:80%) @ 0.7mL/min
Running Time 10 min
Cleaning Procedures
Extensive cleaning of cartridge/column/system with ACN-IPA-Methanol
Instrument AB Sciex QTRAP 6500
To improve the separation, reduce the background, and maintain the method
robust/productive
Method Development/Optimization: 1. Development of A New Sensitive Measurement Method for PFASs in Serum (NJDOH Method)
NJDOH Method (2016)All 12 analytes are baseline-separated and resolved (>0.3 min)
http://dx.doi.org/10.1016/j.chroma.2016.11.063
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Method Development/Optimization: 2. A Validation Study for PFASs in Drinking Water @NJDOH
Based on EPA Method 537 ver. 1.1 (2009), specifically • To achieve practical quantitation levels (PQLs) for PFNA (<5 ng/L) and PFOA (<6
ng/L);• To demonstrate the ECLS has ability and capacity; and• To assist current NJDOH BM projects
Target Analytes: 14 PFASsLinear Range: 5-200 ng/LAccuracy/Precision: Recovery of 70-130% & <20% in RSDLimit of Detection/Quantitation: LOD<1 ng/L & LOQ<5 ng/LStability: testing up to 14 (prior to extraction) and 28 days (after extraction) in a refrigerator (7±3 °C)
Aims:
Objectives:
NJ Department of Health
1.040.80
0.67 0.77
1.34
3.21
0.89
4.99
1.90
0.87
0.50
1.79
1.45 1.35
0.57 0.55
0.10
0.63 0.71
3.83
0.48
4.62
2.79
4.71
0.190.44
0.600.79
0
1
2
3
4
5
6
PFAA
Con
cent
ratio
n (n
g/L)
LOD/LOQ /MRL BY EPA METHOD 537 AT NJDOH-ECLS
LODLOQMRL
LOD=2.82*SD of 10 replicates spiked at 2 ng/L (note: 2.82 obtained from t-distribution of 9 DF at 99%); LOQ=5*LOD*MRL is determined by calculating either 3*AVG or 3*SD of 12 de-ionized water samples, whichever is greater.
Analyte LOD(ng/L)
LOQ(ng/L)
MRL (ng/L)
NEtFOSAA 0.21 1.04 0.57NMeFOSAA 0.16 0.80 0.55PFBS 0.13 0.67 0.10PFDA 0.15 0.77 0.63PFDoA 0.27 1.34 0.71PFHpA 0.64 3.21 3.83PFHxA 0.18 0.89 0.48PFHxS 1.00 4.99 4.62PFNA 0.38 1.90 2.79PFOA 0.17 0.87 4.71PFOS 0.10 0.50 0.19PFTA 0.36 1.79 0.44PFTrDA 0.29 1.45 0.60PFUnA 0.27 1.35 0.79
LOD (Limit of Detection)LOQ (Limit of Quantitation) MRL (Minimum Reporting Level)*NJDEP’s practical quantitation levels (PQLs) for PFNA and PFOA in DW are 5 and 6 ng/L, respectively.
2. A Validation Study for PFASs in Drinking Water @NJDOH: Determination of LODs/LOQs/MRLs for EPA Method 537
*NJDEP’s PQLs for PFNA and PFOA in DW are 5 and 6 ng/L, respectively.
NJ Department of Health
NJDOH BM Project 1: Environmental Contaminant Levels in Blood and Urine Specimens from New
Jersey Clinical Laboratories and Blood Banks
Objectives Determine environmental contaminant levels among NJ
residents (20-74 years old) using remnant clinical laboratory and blood bank specimens.
Establish the state-wide biomonitoring database to screen for disparities.
Compare the NJ levels to national average (e.g., NHANES). Demonstrate laboratory capability/capacity to conduct
biomonitoring studies.
NJ Department of Health
NJDOH BM Project 1 – Study Plan
Sample Size for PFAS Analysis• Target: PFASs in 500 serum specimens• Collected: 376 (as of 5/19/2017)
Serum Collection o NJ-based clinical laboratories and blood banks (Bioreference,
Trenton Community Blood Center, Bergen Community Blood Services)
o Demographic information• Age• Gender• Geographic identifier• Race/Ethnicity (if available)
NJ Department of Health
NJDOH BM Project 1 – Subjects by Demographics
Male51%
Female49%
GENDER
20-3931%
40-5944%
60-7425%
AGE GROUP
White77%
Hispanic7%
Black5%
Others7%
N/A4%
RACE
NJ Department of Health
NJDOH BM Project 1 – Subjects by Residence County
To date, over-sampled from North. More specimens obtaining from Central/South.Later normalized by population size in reporting means (e.g., proc surveymeans in SAS)
NJ Department of Health
aPFASs (ng/mL)Project 1 - NJ Biomonitoring Project (2016) (N=161) 2016 eLatest NHANES (2013-2014)
bRL cGM 50% 75% 90% 95% dGM GM 50% 75% 90% 95%
Et-PFOSA-AcOH 0.028 N/A <RL <RL <RL 0.03 - <LOD <LOD <LOD 0.11
Me-PFOSA-AcOH 0.027 0.07 0.06 0.12 0.24 0.39 - <LOD 0.20 0.40 0.60
PFBuS 0.043 N/A <RL <RL 0.06 0.07 - <LOD <LOD <LOD <LOD
PFDeA 0.096 0.21 0.19 0.29 0.68 1.40 0.14 0.19 0.20 0.30 0.50 0.70
PFDoA 0.066 N/A <RL <RL 0.12 0.31 - <LOD <LOD 0.10 0.20
PFHpA 0.055 N/A <RL 0.08 0.17 0.26 - <LOD <LOD 0.10 0.20
PFHxS 0.096 1.17 1.20 2.18 3.38 4.10 1.22 1.35 1.40 2.40 4.10 5.60
PFNA 0.039 0.77 0.76 1.01 1.33 1.68 0.52 0.68 0.70 1.00 1.60 2.00
PFOA 0.072 2.05 2.04 2.92 4.20 5.39 1.70 1.94 2.07 3.07 4.27 5.57
PFOS 0.071 3.28 3.61 5.05 6.40 7.68 3.55 4.99 5.20 8.70 13.9 18.5
PFOSA 0.018 N/A <RL <RL 0.03 0.05 - <LOD <LOD <LOD <LOD
PFUnA 0.028 0.08 0.08 0.15 0.25 0.34 - <LOD 0.20 0.30 0.50
NJDOH BM Project 1 – Comparison with the latest NHANES data
a<RL data are substituted with RL/√2.bRL is defined as 5*LOD for each analyte.cGMs are provided if >RL measurements are 60% or more.dEstimated GMs for US population in 2016 from NHANES data (1999-2014).eEt-PFOSA-AcOH and PFOSA are no longer measured at CDC after 2012; Thus, the NHANES data provided here is from the last survey period (2011-2012).
NJ Department of Health
NJDOH BM Project 2: Assessing PFNA Body Burdens Following Drinking Water InterventionBackground In 2012-2014, elevated PFNA was detected in public drinking
water in Paulsboro and West Deptford, NJ Discharges from local industrial facilities are potential sources
of PFNA contamination Interventions were implemented for the communities at
different times across past 2 years However, no study is being conducted to systematically
determine: The people were significantly exposed to?What temporal trends over years? How effective the implemented interventions?
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NJDOH BM Project 2 – PFNA-contaminated DW in Paulsboro/West Deptford, NJ
NJ Department of Health
NJDOH BM Project 2 – Where are Communities & Sources?
NJ Department of Health
NJDOH BM Project 2 – Study Objectives & PlanSubject Recruitment Lived in affected areas >2 years Consumed drinking water with
PFNA >10 ng/L Healthy adults, aged 20-74 Subjects #: 101-180, depending on
funds
Sample Collection 2-3 blood draws (~10 mL each)
from each participant One drinking water sample from
each home Questionnaires (for demographic
information and PFAS exposures)
Primary Objectives Determine if the residents have
higher PFNA serum levels than the general population.
Evaluate the effectiveness of interventions by monitoring PFNA serum concentrations over time.
Determine other 11 PFASs.
Exploratory work Estimate the half-life of PFNA in
the body.
Estimate serum:drinking water ratios for PFNA.
NJ Department of Health
Challenges• Matrix Effect: direct injection
of serum → column clogging & peak broadening
• Pre-filtering of the prepared sample
• A guard column (XDB-C8, 4.6x12.5, 3.5-µm)
• Stronger acetic/formic acid solutions (~1%)
• PFASs are mix of branched & linear forms
• Modify existing methods with new branched+linear standards.
• Apply more mass accurate instrument (e.g., QToF-MS/MS).
Future Research Directions
NJ Department of Health
References1. Buck et al., 2011. Integrated Environmental Assessment and Management, Vol. 7, No. 4, 513-541.2. Martin et al., 2010. Journal of Environmental Monitoring, Vol. 12, 1979-2004.3. Benskin et al., 2010. Reviews of Environmental Contamination and Toxicology, Vol. 208, 111-160.4. Olsen et al., 2007. Environmental Health Perspectives, Vol. 115, No. 9, 1298-1305. 5. Post et al., 2012. Environmental Research Vol. 116, 93-117. 6. Oliaei, et al., 2013. Environmental Science and Pollution Research, Vol. 20, 1977-1992.7. Jahnke and Berger, 2009. Journal of Chromatography A, Vol. 1216, 410-421.8. Prevedouros et al., 2006. Environmental Science & Technology, Vol. 40, No. 1, 32-44.9. Bartell et al., 2010. Environmental Health Perspectives, Vol. 118, No. 2, 222-228.10. Seals et al., 2011. Environmental Health Perspectives, Vol. 119, No. 1, 119-124.11. Brede et al., 2010. International Journal of Hygiene and Environmental Health, Vol. 213, 217-223.12. Zhang et al., 2013. Environmental Science & Technology, Vol. 47, 10619-10627.13. MDH, 2013. East Metro PFC Community Updates- Community Meeting, Environmental Public
Health Tracking and Biomonitoring, Minnesota Department of Health, May 15, 2013.14. Yu et al., 2017. Journal of Chromatography A, Vol. 1480, 1-10.
NJ Department of Health
Acknowledgements
NJDOH-PHEL, Onesia Bishop
ECLS, Bahman Parsa,(PI)CT Lab: Zhihua (Tina) Fan, Marilou Palencia, Chris Hargrave,Bhupendra Patel, Mounir SaadInorganic lab: Eric Bind, Douglas Haltmeier, Jhindan Mukherjee, Organic lab: C. David Riker, Norman Patterson, Songyan DuSample Receiving: Susan Muscato
--Support from other DOH divisions
CDC Biomonitoring Grant:U88EH001151
NJ Department of Health