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NEW ADVANCES IN PASSIVE SAMPLING FOR SEDIMENT RISK ASSESSME NEW ADVANCES IN PASSIVE SAMPLING FOR SEDIMENT RISK ASSESSME

NEW ADVANCES IN PASSIVE SAMPLING FOR SEDIMENT RISK ASSESSME - PowerPoint Presentation

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NEW ADVANCES IN PASSIVE SAMPLING FOR SEDIMENT RISK ASSESSME - PPT Presentation

Upal Ghosh Department of Chemical Biochemical amp Environmental Engineering UMBC SETAC HDC Oct 7 2015 Legacy contaminants in exposed sediment contaminates the food chain through ID: 408831

passive sediment pcb dissolved sediment passive dissolved pcb amp freely water sampling concentration concentrations sampler equilibrium fish predicted sediments

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Slide1

NEW ADVANCES IN PASSIVE SAMPLING FOR SEDIMENT RISK ASSESSMENTUpal GhoshDepartment of Chemical, Biochemical, & Environmental Engineering UMBC

SETAC HDCOct 7, 2015Slide2

Legacy contaminants in exposed sediment contaminates the food chain through: bioaccumulation in benthic organismsflux into the water column, and uptake in the pelagic food web.Contaminated sediment

1

Bioaccumulation of Hydrophobic Compounds

P

redictions work reasonably well for natural systems

Predictions become more challenging for industrially impacted sedimentsSlide3

3

2 L water

100g fish

0.0002

mg DDD

1.7

mg DDD

Sediment

1 ppm

K

oc

= 151,000

Large fish

1.7 ppm

Small fish

0.5 ppm

Plankton

0.0265 ppm

Water

0.0001 ppm

Bioaccumulation And Exposure of DDDSlide4

Ehlers and Luthy, ES&T 2003Slide5

Measurement of HOCs in

Water

is

Challenging

Need to measure <ng/L concentrations in sediment

porewater

Two approaches to get to this concentration:Modeling based on partitioning calculations:Sediment concentration and fraction OCModel presumes a certain partitioning behavior for the OCComplication from the presence of BCDifficult to characterize BC partitioning

Direct measurement:Detection limits associated with manageable grab samplingSeparation of colloids challengingPassive samplingSlide6

Carbon Type Influences PAH Partitioning in MGP SedimentsRed line shows predicted Koc based on NOM partitioningMeasured Koc higher by two orders of magnitudePAH association with coal, coke, pitch, or soot increases observed KocSlide7

7Organic Carbon Types in Soil/SedimentSediment contains sand, silt, clays, charcoal, wood, char, coal, & shellsPCBs/PAHs bound to carbonaceous particles less bioavailable

charcoal

coal

sand

wood

shell

char

Petrography images

coal

charcoal

coke

Phenanthrene

partitioning for various organic materials

From:

Ghosh

et al. Environ. Sci. Technol. 2003Slide8

Hydrophobic chemicals partition among the aqueous and different solid phases

Equilibrium distribution can be described by:

Freely dissolved

Passive sampler

DOC

POC

Two approaches to measure total and freely dissolved concentrations:

Remove POC by centrifugation, measure total dissolved concentration and DOC, estimate freely dissolved concentration.

Use calibrated passive sampler to measure freely dissolved concentration, measure DOC/POC, and estimate total dissolved concentration.

Conceptual Understanding of Passive Sampling:

C

total

=

C

free + DOC*KDOC*Cfree + POC*KPOC*CfreeSlide9

PAH & PCB

Uptake Kinetics in Well Mixed Batch

Hawthorne et al.

Analytical Chem

. 2009 & 2011

Under well-mixed conditions

POM, PE, or PDMS reaches close to equilibrium in <30 days

Used to measure site-specific partition constantsSlide10

10Polymer Partition Constants

PDMS

PAH:

log

K

PDMS

-w

= 0.725

log

K

ow

+ 0.479 (

R

2

= 0.99)PCB: logKPDMS-w

= 0.947logKow – 0.017 (R2 = 0.89)POLYETHYLENE

PAH: logKPE-w = 1.22logKow – 1.36 (R2

= 0.99)PCB: logKPE-w = 1.18logKow – 1.26 (R

2 = 0.95)POLYOXYMETHYLENEPAH: logKPOM-w

= 0.839logK

ow + 0.314 (R

2 = 0.97)

PCB: logKPOM-w = 0.791logKow + 1.02 (R2 = 0.95)

The most important parameter necessary for calibration is KpwAccurate measurement of Kpw

for high Kow compounds is challengingA list of provisional Kpw values are available in Ghosh et al. 2014

Common polymers : Polyethylene (PE), Polyoxymethylene (POM) and Polydimethylsiloxane (PDMS)Slide11

11Practical guidance on the use of passive sampling methods (PSMs) for Cfree

for improved exposure assessment of hydrophobic organic chemicals in sediments.

Based on SETAC

Technical Workshop “Guidance on Passive Sampling Methods to Improve Management

of Contaminated

Sediments

,” 2012Practical Guidance for Passive SamplingSlide12

Passive sampler uptake slow in static field deployments12

 

Polymer-water partitioning coefficient

United States Environmental Protection Agency. (

2012, Dec).

Guidelines for using passive samplers to monitor organic contaminants at superfund sediment sitesSlide13

Diffusive Process of HOCs Into PolymersFirst order mass transfer models

=

 

13

Cp

Ku

Ke

Cw

Cw

 

A function of overall mass transfer coefficient

Dissipation of Performance Reference Compounds

X

Cw

Cw

Cp

Diffusion

based models

 

 

D

p

=Diffusion coefficient in polymer, ε = porosity, ρ = particle bulk density D = effective diffusion coefficient, Kd= sediment-water partitioning coefficientSlide14

Tracking pyrene diffusion with Fluorescence 14

PE/POM rod in Saturated Pyrene solution

Aluminum foil

Fluorescence intensity

Distance (mm)

Fluorescence image of polymer slice

CutSlide15

15

Pyrene diffusion into PE (static

)

Sediment side

polymerSlide16

Performance Reference CompoundsEquilibrium slow for: 1) high Kow; 2) static porewaterMass transfer in sediment side difficult to predict

Performance Reference Compounds (PRCs) are used to correct for non-equilibrium

PRCs have similar diffusion properties as

analytes

16

Passive sampler

Time (days)

Polymer fractional uptake

 

 Slide17

Limitations of PRC-correction methodsLow fractional loss of high molecular weight PRCsExtrapolation from low molecular weight PRCs difficult: 17Loss of low molecular weight PRCs

Cfree High molecular weight analytes

Adjustment methods

Inaccurate for high molecular weights

Diffusion model & K

d

-

K

ow

correlation

2

1

st

order model & molar volume correlation

11- Booij, K.; Hoedemaker, J. R.; Bakker, J. F.

Environ. Sci. Technol. 2003, 37 (18), 4213–42202-Fernandez, L. A., C. F. Harvey, and P. M. Gschwend, 2009a. Environmental Science & Technology, v. 43, p. 8888-8894.Slide18

How Do You Use Freely Dissolved Concentrations in Porewater (Cfree) ?

DO NOT: Call it : Bioavailable concentration or Bioavailable fraction

Need a robust toxicity or

biouptake

model to plug in

C

freeFor PAHs: Can plug directly into toxic units calculation based on the narcosis modelFor other bioaccumulative compounds need to plug into a bioaccumulation modelExamples in last talk by Huan XiaSlide19

Ex-situ equilibrium measurements of sediment porewaterIn-situ probing to assess ambient contaminant concentrations or to assess changes with time or with treatmentPictures of typical applications:

sediment

water

Applications of Passive Sampling

Laboratory batch equilibrium

Field evaluation of treatment performance

Depth profiling of

porewater

conc. in sediment

Passive sampling of

porewater

and in-situ bioaccumulationSlide20

Tool for inserting passive sampler frame in sediment. The 8’ pole allows deployment from a boat in shallow water sedimentsPassive sampler encased in stainless steel mesh and framed for sediment deploymentUnderwater video camera for confirming placement depth

Rope and buoy for retrieval after deployment

Deployment Device For Inserting Passive Sampler Frame Into Surface Sediments

Image from underwater camera showing the passive sampler being inserted into sediment Slide21

Figure 1. Chronic toxicity to H. azteca (28-day) can not be predicted from total PAH concentration in MGP sediment

Figure 2. Chronic toxicity to H. azteca

(28-day) can be predicted by estimating PAHs in sediment pore water.

Prediction of

Toxicity

:

Sediment vs. Freely Dissolved Conc.

Kreitinger et al , ETC 2007Slide22

Prediction of Biouptake in benthic organisms:

Sediment vs. Freely Dissolved Conc.

7 freshwater and marine sediments

Freely dissolved conc. measured by passive sampling and also directly

Lipid concentrations better predicted from freely dissolved

porewater

Werner et al. ES&T 2010

Predicted from sedimentPredicted from porewaterSlide23

Sediment

Passive samplers

Water flow in aquaria tanks

Components in each aquaria

Treatments

:

Clean sediment (Rhode River)

PCB

impacted

sediment (Near-shore Grasse River)

PCB

impacted sediment-AC

treated in the lab

Replicate

aquaria with passive samplers in water column and sedimentFish species: ZebrafishPCB-free diet

Sampling after 45 and 90 days23Prediction of PCB Uptake in FishFadaei et al. ES&T 2015Slide24

24Sediment Partitioning Coefficient Predictions

 

Schwarzenbach

et al. 2003

 

Werner et al. 2009

 

 Slide25

The total PCB concentration in fish was decreased by 87% after treatment with AC25PCB Residue in Zebrafish

after 90 DaysSlide26

Steady-State Approach

Kinetic

Approach

 

26

k

1

k

2

k

e

Predicting PCB Uptake in Fish

=

- (

+

)

=

 

(

Arnot

and

Gobas 2004)Slide27

Observed and predicted PCB concentrations in fishEquilibrium modelKinetic model

with ingestionSlide28

ACKNOWLEDGMENTSFunding support from SERDP/ESTCP programs, NIEHS, USEPA GLNPO, and AlcoaSeveral students and post docs

KEY MESSAGES

Freely dissolved concentrations of HOCs good predictor of

biouptake

and toxicity

Passive samplers can accurately measure freely dissolved

concentrations at equilibriumCorrections needed for non-equilibrium for in-situ measurementsSlide29
Slide30

30

Extraction Device

a

lso containing a lipid source

(sunflower oil) to mimic the lipophilic environment

Phase one: acidic gastric condition

Phase two: near-neutral intestinal condition

Simulated gastrointestinal fluid

CARBON TYPE ALSO INFLUENCES PAH BIOAVAILABILITY IN ANIMAL GUT

SERDP FUNDED STUDYSlide31

31COMPARISON BETWEEN SOIL KD & BIOACCESSIBILITYSlide32

BACKGROUND ON ESB GUIDANCE (2003, 2008)ESBs are based on a target lipid model (Di Toro et al. 2000)Developed critical lipid concentrations for 49 aquatic species 5th percentile expected to be protective of95 percent of species tested

Genus Mean Acute Value (mmol/g octanol)

Percentage Rank of GeneraSlide33

TIERED ASSESSMENTSlide34

PAH AND PCB ABSORPTION EFFICIENCY IN CLAMSFrom: McLeod et al. Environ. Sci. Technol. 2004

Tracking 3H-BaP and 14C-2,2’,5,5’ PCB through a clamSlide35

ESB GUIDANCES (2008, 2005)