DNAPL Source Zones - Contaminated Site Clean-Up ...
Transcript of DNAPL Source Zones - Contaminated Site Clean-Up ...
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DNAPL Source Zones
Mark L. Brusseau University of Arizona
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Superfund Basic Research Program University of Arizona
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(NIEHS), an institute of the National Institutes of
•
contamination
Funded and administered by the National Institute of Environmental Health Sciences
Health (NIH)
Hazardous wastes investigated include: arsenic, chlorinated hydrocarbons, and mine tailings
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The DNAPL Problem
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•
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Primary Source of Contaminant Mass
Site Characterization
Remediation
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The Source-Zone Issue
that is the question… To Remediate or Not To Remediate---
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Recent Studies
• 2002. DNAPL Source Reduction: Facing theChallenge.
• 2003. The
• 2004.
.
Interstate Technology and Regulatory Council.
Environmental Protection Agency. DNAPL Remediation Challenge: Is There a Case for Source Depletion?
National Research Council. Contaminants in the Subsurface: Source Zone Assessment and Remediation
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Summary
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Complete Mass Removal Not Possible
Is Partial Removal [Mass Reduction] Beneficial?
Need To Define Objectives
Cost/Benefit Analysis
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Key Questions
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•
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Expected Degree of Mass Reduction?
Impact of Specified MR on Mass Flux?
Impact of Mass Flux Reduction on Risk?
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Answers
• Need to Understand the Impact of Source-zone Architecture and Dynamics on Mass Flux Behavior
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Research Needs • SERDP/ESTCP
of Chlorinated Solvent Sites. 2001.
–
– Processes
–
Expert Panel Workshop on Research and Development Needs for Cleanup
Focus Research on Source-Zone Issues
Source-zone Architecture and Mass Transfer
Pore-scale Processes
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Research Needs
•
– between mass reduction and mass flux
– multiple (pore, column, intermediate, field) scales
– Distribution and mass-transfer behavior of DNAPLs in heterogeneous (low-permeability or fractured) systems
UA/SBRP Expert Panel DNAPL Workshop. 2005.
Source-zone mass flux processes, and the relationship
Distribution and mass-transfer behavior of DNAPLs at
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Continued
– of aging and the relative contributions of trapped
dissolved mass
–
(real-world) settings
– associated upscaling
Long-term mass flux behavior, including the influence
DNAPL, sorbed mass, and matrix-associated
Impact of co-contaminants on phase properties (wettability, interfacial tension) in complex, natural
Mathematical modeling at multiple scales, and
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Mass Flux
Source Zone
Contaminant Flux
High Concentration
Low Concentration Source Zone
ContaminantFlux
High Concentration
Low Concentration
High Concentration
Low Concentration
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Flux Reduction vs. Mass Removal
0
1
0 100
l (%)
i
I l
I l
13
0.25
0.5
0.75
25 50 75
Mass Remova
M a s
s Fl
ux R
edu c
to n Non- dea Mass Transfer
dea Mass Transfer
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Factors Influencing Mass Flux
• ield Dynamics
•
•
•
Flow-F
DNAPL Distribution and Configuration
Dissolution Dynamics
Mass Transfer and Transformation Processes
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Measuring Mass Flux
• lux in the Field
•
Measuring Mass F
Lynn Wood Presentation
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Predicting Mass Flux Reduction
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•
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Flux Reduction-Mass Removal Relationships
Understand Impacts of Source-zone Architecture and Dynamics on Mass Flux
Priority Research Need
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Intermediate-Scale Experiments
• • • •
• •
Examine Heterogeneous Systems Permeability Variability Non-uniform NAPL Distribution Multiple Mass-transfer Processes
Controlled/Well-defined Systems Evaluate Flux vs. Mass Removal Behavior
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UA-PNNL Experiments •
– – –
• saturation in-situ (mass removal)
• i– – –
Multiple methods to measure aqueous concentrations (mass flux):
Depth specific ports [e.g., multilevel sampling ports] Vertically integrated ports [e.g., fully screened MWs] Flow-cell effluent [e.g., extraction well]
Dual-energy gamma system to measure NAPL
Additional characterizat on methods: Non-reactive tracer test Dye tracer test Visualization of dyed TCE
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Flow-cell Schematic
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Flow Cell
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TCE Concentrations
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Mass Flux-Mass Removal
0
1
0
n
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
20 40 60 80 100
Mass Removed (%)
Mas
s Fl
ux R
educ
tio
Sand- Well Sorted Sand- Poorly Sorted
Homogeneous P.M., Uniform NAPL
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Mass Flux-Mass Removal
0
1
0
(%)
i
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
20 40 60 80 100
Mass Removed
Mas
s Fl
ux R
educ
tion
Homogeneous P.M. Un form NAPL Heterogeneous P.M. Non-uniform NAPL
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Pore-scale Research
• – – – –
• – –
Topics: Multi-phase Fluid Displacement Wetting/Non-wetting Fluid Distributions Fluid-Fluid Interfacial Areas Mass-transfer Processes
Methods: High-Resolution Imaging--- MRI/NMR; X-ray Pore-scale Modeling--- Network, Lattice-Boltzmann
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GeoSoilEnviroCARS
• research facility at theAdvanced Photon Source, Argonne, IL
• DOE, State of Illinois
Synchrotron-based
Supported by NSF,
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Synchrotron X-ray CT Images
NAPL = white
Solids = dark gray, Water = black,
Solids = gray, Water = blue, NAPL = red
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Examples of NAPL Ganglia
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Time Series
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Acknowledgements
•
• McColl, Michele Mahal, Mart Oostrom
NIEHS SBRP
Greg Schnaar, Justin Marble, Colleen
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A. Lynn Wood Michael C. Brooks
U.S. EPA/ORD/NRMRL
Measurement and Use of Contaminant Flux as an
Assessment Tool for DNAPL Remedial Performance
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in the Field Methods:
¾ Multi-Level Sampler (MLS) Transects ¾
¾ ) ¾ Integral Pumping Test (IPT) ¾
Measuring Contaminant Mass Flux
Passive Flux Meters (PFM) Horizontal Flow Treatment Wells (HFTWs
Modified Integral Pumping Test (MIPT)
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et al
Contaminant Flux Estimates by MLS Transects
(from Newell ., 2003)
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MLS Transect Method
• – i
– – ll l–
• – – – –
Advantages: Generates spatial informat on on concentration distributions Methods exist to estimate uncertainty Sma waste vo umes produced Conventional
Disadvantages: Requires independent estimation of water flux Contaminant measures are instantaneous Interrogates small volumes of aquifer Data must be spatially integrated to obtain contaminant mass flows
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Well
lWell
Contaminant Mass Flux Measurements by Horizontal Flow Treatment Wells ( HFTWs )
(from Huang et al. 2004 and Goltz et al. 2004)
Downflow
Upf ow
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(HFTW) Method
• – – – – –
• –
) – – – –
Horizontal Flow Treatment Well
Advantages: Generates water flux and contaminant mass flux estimates Interrogates large volumes of aquifer Can be used in deep aquifers Does not extract groundwater Can estimate horizontal and vertical aquifer conductivities
Disadvantages: Does not provide spatial information (difficult to quantify uncertaintyAssumes aquifer is homogeneous Uses tracers to estimate interflow Does not function in all wells Underestimates maximum resident contaminant concentrations
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Passive Flux Meters (Hatfield et al., 2004)
Sorbent (with Tracers
(minimize vertical flow)
Tube for flow bypass
Retrieval wire
q = f(depth)
J = f(depth)
activated carbon)
Viton Washers
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Passive Flux Meter Concepts ContaminantWater Flux
q0
Tracer ElutedTracer Remaining
Flux Contaminant Sorbed
(Hatfield et al., 2004)
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Passive Flux Meter Method
• –
– – l – l– – i
• – l–
– –
Advantages: Generates spatial information on cumulative water and contaminant mass flux Methods exist to estimate uncertainty Generates loca estimates of horizontal aquifer conductivity Small waste vo umes are produced Passive Inexpens ve
Disadvantages: Interrogates small vo umes of aquifer Data must be spatially integrated to obtain contaminant mass flows and total water discharge Uses resident tracers to estimate groundwater flux Does not function in all wells
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Integral Pumping Test(Bockelmann et al. 2001, 2003; Schwarz et al., 1998; Teutsch et al. 2000;
Ptak et al. 2000)
Measured mass fluxesat control cross-sectionsPumping tests
ResidualNAPL-phase
Q, C(t)
mass flux
C
t
C
t
Mea
sure
men
ts(f
ield
sca
le)
Fiel
d si
te
Q, C(t)
Comparison andInterpretation
Control
Plane I
flux 1
Control
Plane II
flux 2
Measured mass fluxesat control cross-sectionsPumping tests Measured mass fluxesat control cross-sectionsPumping tests
ResidualNAPL-phase
Q, C(t)
mass flux
C
t
C
t
Mea
sure
men
ts(f
ield
sca
le)
Fiel
d si
te
Q, C(t)
ResidualNAPL-phase
Q, C(t)
mass flux
C
t
C
t
Mea
sure
men
ts(f
ield
sca
le)
Fiel
d si
te
Q, C(t)
Comparison andInterpretation
Control
Plane I
flux 1
Control
Plane II
Comparison andInterpretation
Control
Plane I
flux 1
Control
Plane II
flux 2flux 2
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Integral Pumping Method
• – – –
• – ( l) – – – –
) – –
Advantages: Generates contaminant mass flow estimates Interrogates large volumes of aquifer Can be used in deep aquifers
Disadvantages: Costly wastewater disposaRequires lengthy time execution Assumes aquifer is homogeneous Does not estimate water flux Does not provide spatial information (difficult to quantify uncertaintySubject to the limitations of sampling configuration Underestimates maximum resident contaminant concentrations
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Modified Integral Pumping Test
J = q0c
Interpreted from concentration –time
series
x
y
q0 i
well
Estimate q0 directly from IPT results
Observat on point
Pumping
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Diff
eren
ce in
Ele
vatio
n
Modified Integral Pumping TestSuperposition of Uniform flow and multiple Sink terms
0.00003
0.00002
0.00001
0
-0.00001
-0.00002
-0.00003
∆ φ − = o
T B q ∆ x +
4π T 1 ∑
i = 1
n
iQ
q = o
r i w
r obs [ 2 [
2
ln
∑ ln 4π B ∆ x i = 1
− Q n
At ∆φ = 0,
i ]
]
r i w
r obs [ 2 [
2 i
]
]
0 0.005 0.01 0.015 0.02 0.025 0.03 0.035
Q*ln(ε )
Flux Well 1 Flux Well 2 Flux Well 3
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2) Measure Elevations = f(Q)
1) Measure Q = f(t)
Elev(t0) Elev(Q1)
Q
t
Elev(Q3)Pumping Well Observation Well
Elev(Q2)
Modified Integral Pumping Test
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Modified Integral Pumping Method
• – – – –
• – ( l) – – –
) – –
Advantages: Generates contaminant mass flow estimates Interrogates large volumes of aquifer Can be used in deep aquifers Estimates water flux
Disadvantages: Costly wastewater disposaRequires lengthy time execution Assumes aquifer is homogeneous Does not provide spatial information (difficult to quantify uncertaintySubject to the limitations of sampling configuration Underestimates maximum resident contaminant concentrations
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Assessing DNAPL Source Remediation Performance
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Source Remediation = Contaminant Flux Management
Pre-Remediation: Control
c)
Control
c)
Post-Remediation:
Jc=qw•C
Most contaminated
Least contaminated
Source Zone
Plane
Contaminant Flux (J
Source Zone
Plane
Contaminant Flux (J
Flux = Flow • Concentration
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Pre-Remediation:
Dissolved Plume
DNAPL
DNAPL
DNAPL
MASS DEPLETION RESPONSE
Source Zone
Control Plane Compliance Plane
Dissolved
Partial Mass Removal + Enhanced Natural Attenuation:
Source Zone Plume
Dissolved
Partial Mass Removal:
Source Zone Plume
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Field Demonstrations
Laboratory Experiments
Mathematical Modeling
Impacts of DNAPL Source Zone Treatment: Experimental and Modeling Assessment of
Benefits of Partial Source Removal
…assess the benefits of aggressive in situ DNAPL source-zone remediation
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Project Team
• • •
l Air Force Institute of Technology • • •
Mike Annable – University of Florida Michael Brooks – EPA/ORD/NRMRL Ron Falta – Clemson University
• Mark Go tz – Jim Jawitz – University of Florida Suresh Rao – Purdue University Lynn Wood – EPA/ORD/NRMRL
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DNAPL Field Sites 99
999
9/
99
Fort Lewis, Washington Pre-Remedial Flux 10/03 Resistive Heating 12/03-8/04 Post-Remedial Flux 8/05
Hill AFB, Utah Pre-Remedial Flux 5/02 Surfactant Flushing 6/02 Post-Remedial Flux 6/03&10/04
CFB, Canada Pre-Remedial Flux 5/04&7/04 In-situ Chemical Oxidation 6 05 Post-Remedial Flux 4/06
Jacksonville, Florida Pre-Remedial Flux 6/04 Cosolvent Flushing 6-7/04 Post-Remedial Flux 5/06
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Nor
thin
g (fe
et)
lls
iWells
ii i
Hill AFB OU2
293070
293090
293110
293130
293150
293170
Flux We
Observat on
Approx mate Flow D rect on
U2-154
U2-153
U2-117
U2-216
U2-155
U2-157
U2-152
U2-150
U2-148
U2-116
U2-149
U2-151
Layton, Utah
1870620 1870640 1870660 1870680 1870700 1870720
Easting (feet)
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1
10
1
10
1
10
100
0
TCE Concentration Time Series
TC
E C
once
ntra
tion
(mg/
L)
Elapsed Time (Hours)
May ‘02
q0
q0
q0
100
1000
100
1000
0.1
20 40 60 80 100
Jun ‘03
Oct ‘04
U2-154
U2-152
U2-150
U2-148
U2-116
U2-149
U2-151
U3-153
U2-155
U2-157
= 1.7 cm/d
= 2.9 cm/d
= 3.2 cm/d
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l
C
C
t
t
Adapted from Bockelmann et al. (2003)
Interpretation of CT series
Pumping well
Plume boundary
Pumping wel
Plume boundary
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May '02 Jun '03 Oct '03
Hill AFB OU2 Layton, Utah TCE Flux Summary 10
TC
E F
lux
(g/s
quar
e m
/day
)
1
0.1
0.01 154 152 150 148 116 149 151 153 155 157
Flux Well
56
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0 10 20 30 40 50 60 70 80 90
0 10 20 30 40 50 60 70 80 90
57
i l
0
1
2
3
4
5
6
7
8
9
10
154 152 150 116 151 153 157
154 152 150 116 151 153 157
Well
Flux Meter - Darcy Velocity (cm/day)
Ele
vatio
n (f
eet) 4660
4665
4670 Pre Remedial Flux Measurement Test May 2002
Second Post Remed al F ux Measurement Test October 2004
4660
4665
4670
148 149 155
148 149 155
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0 10 20 30 40 50 60 70 80 90
0 10 20 30 40 50 60 70 80 90
58
4660
4665
4670
4660
4665
4670
-4
-3.5
-3
-2.5
-2
-1.5
-1
-0.5
0
0.5
1
1.5
2
154 152 150 116 151 153 157
154 152 150 116 151 153 157
Flux Meter – Log TCE Flux (gram/square meter/day)
Ele
vatio
n (f
eet)
Second Post Remedial Flux Measurement October 2004
Pre Remedial Flux Measurement May 2002
148 149 155
148 149 155
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0
1
2
3
4 (
Hill AFB OU2 Darcy Velocity Comparison
May 2002 June 2003 Oct 2004
PFM MIPT PFM PFMMIPT MIPTD
arcy
Vel
ocity
cm/d
ay)
Layton, Utah
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Well-Averaged Flux Summary
0.001
0.01
0.1
1
10
0.001 0.01 0.1 1 10
lux (g / m2 / day)
l2 /
day)
IPT F
FM F
ux (g
/ m
TCE 5/02
TCE 6/03
DCE 6/03
TCE 10/04
DCE 10/04
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NAPL Area 1
NAPL Area 2
NAPL Area 3
Fort Lewis EGDY Area 1 Source Zone of Ft. Lewis Plume
Tacoma, Washington
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B09
Fort Lewis EGDY Area 1
5,216,710
5,216,720
5,216,730
5,216,740
5,216,750
5,216,760
5,216,770
5,216,780
536,390 536,400 536,410
LC-213 LC-214
LC-212
C08 LC-211
LC-207
LC-206
LC-205
LC-209
LC-204
D14
LC-210
LC-203
LC-208
LC-202
LC-215
LC-201
Tacoma, Washington
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10
20
63
0
0
1
2
PFM Velocity Field (cm/hr) University of Florida
Fort Lewis EGDY Area 1
33
13
Dep
th (f
t bgs
)
23
20 40 60 80 100 120 140 160 180
0.2
0.4
0.6
0.8
1.2
1.4
1.6
1.8
2.2
2.4
2.6
2.8
Tacoma, Washington
Distance along transect (ft)
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10
20
64
0
0 100 120 140 160 180
-2 hr-1) University of Florida
Fort Lewis EGDY Area 1
33
13
Dep
th (f
t bgs
)
23
-0.005
0.005
0.01
0.015
0.02
0.025
0.03
0.035
0.04
0.045
0.05
0.055
0.06
0.065
0.07
20 40 60 80
PFM TCE Flux (mg cm
Tacoma, Washington
Distance along transect (ft)
Range: <0.1 to 20 g/ sqm /day; Transect average 2 g / sqm / day.
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Fort Lewis EGDY Area 1
Flux Well
-1)
Tacoma, Washington
Ft Lewis Modified Integrated Pump Test - Oct/Nov 2003
0.01
0.10
1.00
10.00
100.00
201 202 203 204 205 206 207 211 212 213
Dar
cy F
lux
(cm
hr
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Fort Lewis EGDY Area 1
0.01
0.1
1
10
201 202 203 204 205 206 207 211 212 213
TCE
Flux
(g m
-2 d
-1 )
IPT
Average Pre-Remedial Flux, Oct/Nov 2003 Tacoma, Washington
0.0001
0.001
Flux Well
PFM
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•
• in flux at Hill AFB
• methods to date are comparable
Summary
Modified IPT method is being used to measure pre- and post-remedial flux Approximately an order of magnitude decrease
Flux estimates based on flux meter and IPT
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Acknowledgements
•
• Research and Development Program (SERDP)
Onsite Assistance – Hill AFB EMR/URS, Utah – LFR, Florida – US Army Corps of Engineers Seattle
District/Fort Lewis Public Works, Washington – University of Waterloo, Canada
Project Funding: Strategic Environmental
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