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Article history:
Received 17 April 2012
Received in revised form
2 July 2012
Accepted 1 August 2012
Available online 15 September 2012
A comparative life cycle assessment is presented for four different management options for a trichloroethene-contaminated site with a contaminant source zone located in a fractured clay till. The
compared options are (i) long-term monitoring (ii) in-situ enhanced reductive dechlorination (ERD), (iii)
in-situ chemical oxidation (ISCO) with permanganate and (iv) long-term monitoring combined with
treatment by activated carbon at the nearby waterworks. The life cycle assessment included evaluation of
both primary and secondary environmental impacts. The primary impacts are the local human toxic
impacts due to contaminant leaching into groundwater that is used for drinking water, whereas the
secondary environmental impacts are related to remediation activities such as monitoring, drilling and
construction of wells and use of remedial amendments. The primary impacts for the compared scenarios
were determined by a numerical risk assessment and remedial performance model, which predicted the
contaminant mass discharge over time at a point of compliance in the aquifer and at the waterworks. The
combined assessment of risk reduction and life cycle impacts showed that all management options result
in higher environmental impacts than they remediate, in terms of person equivalents and assuming
equal weighting of all impacts. The ERD and long-term monitoring were the scenarios with the lowest
secondary life cycle impacts and are therefore the preferred alternatives. However, if activated carbon
treatment at the waterworks is required in the long-term monitoring scenario, then it becomes unfavorable because of large secondary impacts. ERD is favorable due to its low secondary impacts, but only if
leaching of vinyl chloride to the groundwater aquifer can be avoided. Remediation with ISCO caused the
highest secondary impacts and cannot be recommended for the site.
2012 Elsevier Ltd. All rights reserved.
Keywords:
Remediation
Contaminated sites
Groundwater
Life cycle assessment
Chlorinated solvents
Natural attenuation
Chemical oxidation
Enhanced reductive dechlorination
Decision support
1. Introduction
Contaminated sites are usually remediated because they are
assessed to pose a risk to the local environment (groundwater,
surface water, terrestrial ecosystems) and to users of the site
(indoor air risk, risk of direct contact with soil, etc.). The reduction
of the local risks, also termed the primary impacts associated with
a contaminated site, however, is done at the expense of increasing
the secondary impacts on health and the environment. These
secondary environmental impacts are the local, regional and global
impacts arising from the extraction, material, use and end-of-life
phases of all consumables, equipment and energy used for the
remediation, and can be quantied by a life cycle assessment (LCA)
(Lemming et al., 2010a; Morais and Delerue-Matos, 2010). An LCA
also provides a framework where the tradeoff between primary
The model results are then employed with a life cycle assessment to determine the primary and secondary environmental
impacts of each management alternative and thereby evaluate the
overall environmental benet of each alternative. Such information
can be used as the basis for comparison and selection of management options for decision makers. Note that in this assessment we
exclude the evaluation of tertiary impacts, i.e. the environmental
impacts associated with the future use of the site (Lesage et al.,
2007).
2. Materials and methods
2.1. Site description
The concept of combined risk and life cycle assessment is
illustrated for a contaminated site located at Sortebrovej in Tommerup, Denmark (Fig. 2). The site is contaminated by trichloroethene (TCE), which is mainly located in a fractured clay till
between 13 and 23 m below ground surface (mbgs) and in a thin
upper sand aquifer located beneath the clay till. A conceptual
geological model and a transect of the source zone is shown in
Fig. 2. The contamination at Sortebrovej poses a risk to the drinking
water abstraction wells at the Tommerup waterworks where water
is extracted from the regional groundwater aquifer. The water
supply wells are located 200 m northeast of the contaminant
source zone. The remediation targets an 11 m deep treatment zone
which covers a horizontal area of 750 m2 in the clay till and
1500 m2 in the sand. The contaminant mass of TCE was estimated
to 23.4 kg based on source zone calculations (Chambon et al., 2011).
Full scale remediation by in-situ enhanced reductive dechlorination (ERD) was started at the site in 2006 with the addition of
a fermentable electron donor (emulsied soybean oil and lactate)
and specic degrader organisms (Dehalococcoides) to the target
treatment zone in order to stimulate the complete microbial
Timeframe
WW
POC
Inventory of
secondary emissions
and resource use
Accumulated
intake
Concentration
Mass depletion
in the source
Concentration
Mass/flux
Inventory of primary
emissions
Time
Time
Impact assessment
Time
Combined evaluation
etc
393
Normalised impact
Fig. 1. Concept for combined evaluation of remedial performance, risk assessment and life cycle assessment. POC: Point of compliance. WW: Waterworks.
394
Fig. 2. Location of the Sortebrovej site and water supply wells in Tommerup. The transect runs along the groundwater ow direction and shows the initial aqueous TCE
concentrations [mg/L] and the conceptual local geology and fracture setup used in the model. POC: Point of compliance for assessing groundwater quality criteria. The point is
located 100 m downstream of the site.
Due to the large depth to the source zone (>13 m), excavation
followed by ex-situ treatment is not a viable option for this site.
2.3. LCA approach
The functional unit, which denes the service compared in the
life cycle assessment, is dened here to be the management of the
target treatment zone which leads to a 99% removal of the
contaminant mass. The mass removal target ensures that the
Danish groundwater quality criterion for TCE of 1 mg/L is met at the
point of compliance 100 m downstream from the site.
The life cycle assessment considers the extraction of raw
materials, the manufacturing, use and end-of-life phases for
consumables, equipment, energy etc. used in the different
management options (see Fig. 3). In order to simplify the assessment, the materials used for pumps, mixing tanks and containers
for amendments were disregarded as they were assumed to result
in only negligible contributions to impacts due to relatively low
amounts of materials used and the high direct reuse rate. The
uptake of injection wells in the closure phase of the project was
disregarded due to uncertainty of the fate of these wells. If uptake
was included, the impact would be equal for the ERD and ISCO
system, whereas the long-term monitoring scenario would not be
affected. Furthermore, the CO2 emission caused by the degradation
of TCE was excluded from the inventory due to its minor contribution. The Life Cycle Impact assessment method applied was
EDIP2003 (Hauschild and Potting, 2005) for non-toxic impacts and
USEtox (Rosenbaum et al., 2008) for the toxic impact categories.
All results are normalized to person equivalents (PE) by dividing
with the average impact from a European citizen in 2004 (Laurent
et al., 2011a, 2011b).
System
boundary
Raw materials
and energy
395
Table 1
Site properties used for the inventory in Table 2.
Parameter (unit)
Clay till
Sand
750
10
0.3
1.8
75
50
1500
1
0.3
1.8
75
50
210
210
Raw materials
and energy
Raw materials
and energy
Installation of
injection wells
Treatment of soil
from borings
Bentonite
Groundwater
extraction
Steel recycling
(80%)
Injection wells
Pumps
Containers
Gravel
CO from TCE
degradation
Closure and
uptake of wells
Steel
Remedial
amendments
Transport
Injection of
oxidant/ substrate
Transport
HDPE recycling
(80%)
Personnel
transport
Decomposition of
amendments
Monitoring
Production phase
Emissions
Use phase
Emissions
Local toxic emissions
Remedial amendments cover substrate and bacterial culture (ERD) and oxidant (ISCO)
Fig. 3. System boundaries of the life cycle assessment.
End-of-life
Emissions
396
Table 2
Inventory data for amendments added to the subsurface.
Parameter (unit)
ERD low
rate
ERD high
rate
ISCO
3700
65
5500
110
e
e
219
0.18
219
0.18
e
e
e
e
e
e
525
0.21
52,500
average NOD for the site to be 18 kg KMnO4 per tonne of soil in clay
till samples (Hnning and Bjerg, 2003). For the sand aquifer a NOD
value of 1 kg KMnO4 per tonne soil was applied using typical values
for Danish aquifer materials (Hnning et al., 2007a). The carbon
dioxide generated from the reaction between the oxidant and the
soil was included in the inventory and assumed to be released to
the atmosphere. Table 2 lists the inventory data for amendments
used in ERD and ISCO.
The long-term management scenario combined with treatment of the abstracted groundwater at the waterworks uses
granular activated carbon (GAC). An adsorption capacity of 2% (w/
w) was assumed for the adsorption of TCE on to the GAC.
Compared to traditional Danish drinking water treatment with
aeration and sand ltration, adding activated carbon ltration
leads to an increased energy use of 10% or 0.025 kWh per m3
(Cowi, 2009).
Table 3 provides an overview of the activities included in the
LCA of each scenario. More details regarding the energy use for the
drilling of wells, injection and pumping is found in Table A1 in
Supporting Information (SI). The table also shows the material used
per meter well and the amount of activated carbon consumed.
Monitoring activities for all scenarios include transportation
(40 km return), pumping of groundwater and subsequent analyses
in a laboratory. The transportation distances and site visit
frequencies for the scenarios are found in Table A2 in SI.
Table 3
Overview of main activities included in each management scenario.
Long-term monitoring
Monitoring at and
downstream of the sitea
a
b
c
VC concentration (g/L)
25
20
397
15
10
5
0
6
Total concentrations at
100 m
4
3
2
TCE criterion
1
0
0.5
VC concentrations at
100 m
0.4
0.3
VC criterion
0.2
0.1
0.0
0
200
400
600
Time (years)
800
1000
Monitoring
ISCO
Fig. 4. Model results showing the (a) contaminant mass in the treatment zone, (b)
contaminant concentrations at the POC in the groundwater aquifer 100 m downstream
of the source (sum of TCE, DCE and VC), and (c) VC concentrations at 100 m. Note the
different scales on the y-axes.
Table 4
Model-estimated timeframes for mass removal and compliance with groundwater quality criteria at the POC, and model-estimated leached amounts of contaminants to the
aquifer.
Timeframe (years)
Long-term monitoring
ERD (low rate)
ERD (high rate)
ISCO
a
Compliance with
criteria at POC
TCE
DCE
VC
670
200
90
80
830
400
10a
10a
23.2
0.05
0.2
0.007
0
0.3
0.02
0
0
1.1
0.007
0
The monitoring period was set to be 10 years even though the results indicate that there is no exceedance of the quality criteria at the POC.
398
0.35
Total concentrations at
waterworks
0.3
Concentration (g/L)
0.25
0.2
0.15
0.1
0.05
0
0.05
0.04
0.03
0.02
0.01
0.00
200
400
600
Time (years)
800
1000
Monitoring
ISCO
200
Sum
400
600
Time (years)
TCE
800
DCE
1000
VC
Fig. 5. (a) Contaminant concentrations at the waterworks (sum of TCE, DCE and VC), and (b) Individual waterworks concentrations of TCE, DCE and VC for ERD (low rate).
reaction rate occurs in the ERD process, the remediation timeframe is doubled and the environmental impacts are increased by
an average of 70%. Furthermore, the results reveal that
combining the long-term monitoring scenario with activated
carbon treatment at the waterworks will increase impacts of this
scenario by a factor of 8.
3.4. Primary life cycle impacts
Table 5 lists the primary toxic impacts due to human ingestion
resulting from the leaching of contaminants to drinking water. In
the long-term monitoring scenario no source remediation is conducted and so 23.2 kg of TCE will leach to the groundwater leading
to a human toxic (cancer) impact of 15 PE. If source zone remediation is applied with ERD (high rate) or ISCO then this primary
impact is reduced to very low levels (<1 PE). For the low rate ERD,
however, the primary impact is increased to 42.5 PE as a consequence of the remedial action. This is due to the generation and
leaching of the degradation product vinyl chloride (VC), which has
a higher carcinogenic and chronic toxicity than the mother product
TCE. Thus, despite the release of only approximately 1 kg of VC, the
corresponding toxicity is higher than that of the original 23.4 kg of
TCE.
3.5. Environmental hotspots
Fig. 7 shows the contribution to the environmental impacts of
the different sub-parts of the ERD high rate, ERD low rate and
ISCO scenarios. The long-term monitoring scenario is not shown,
1500 PE
625 PE
160
140
120
100
80
60
40
20
0
Global
Warming
Ozone
formation
Acidification
Long-term monitoring
Terrestrial
Aquatic
eutrophication eutrophication
Respiratory
inorganics
ISCO
Ecotoxicity
freshwater
Fig. 6. Life cycle assessment results for the secondary impacts in PE (person equivalents) for the ve compared management options.
Long-term
monitoring
ERD
(low rate)
ERD
(high rate)
ISCO
ea
15
15
7.5
35
42.5
0.1
0.4
0.5
ea
0.15
0.15
399
4. Discussion
4.1. Secondary impacts
The life cycle assessment of the secondary impacts of the
assessed scenarios showed that long-term monitoring and ERD are
the management options that have the lowest life cycle impacts,
even though these options have very extended timeframes.
However, long-term monitoring without actual source removal
results in elevated drinking water concentrations at the waterworks, where activated carbon treatment might be necessary to
ensure safe drinking water. In this case, the environmental impacts
of the long-term monitoring scenario increase by a factor of 8 and
disfavors this option. In this case study, the environmental burden
from the added electricity use at the waterworks was allocated
based on the mass discharge from the contaminated site and the
water volume this would contaminate up to the MCL. This resulted
in a contaminated water volume of 23 million m3, which is
equivalent to 170 years of drinking water production at this
waterworks. If the drinking water was already contaminated above
the MCL due to other contaminated sites, the burden allocated to
this site might be lower. It should also be noted that the assessment
assumes that the current technologies remain valid for the long
duration of the scenarios. This is a conservative assumption as
treatment technologies and electricity production will develop over
time. In the assessment of ERD it was assumed that all methane
generated by the fermentation of the substrate was released to the
atmosphere. This is a worst case assumption. The treatment zone at
the studied site is located 13 m below ground with an extended
unsaturated zone above it. It is therefore likely that a part of the
methane will be reduced by methane oxidizing organisms in the
top soil and this can reduce the impact scores for global warming
and ozone formation signicantly (refer to Fig. 7).
The secondary impacts of ISCO are much larger (by up to a factor
of 16) than those for ERD and long-term monitoring due to the large
amount of oxidizing agent needed. Even though the timeframe for
ISCO is long due to the mass transfer limitations in the clay till, the
impacts due to site visits for monitoring and injection are minor
when compared with that due to the oxidizing agent. This nding is
consistent with the LCA study by Cadotte et al. (2007) who studied
alternatives for groundwater remediation of diesel oil including
ISCO with Fentons reagent. Here large amounts of Fentons reagent
(14,250 tonnes) generated considerable secondary impacts due to
its production. Sodium persulfate (Na2S2O8) is an alternative
oxidant for chemical oxidation. For this site a persulfate demand of
300 tonnes was estimated based on an average clay till NOD of
11 kg Na2S2O8/tonne determined in laboratory batch tests
(Hnning and Bjerg, 2003) and a NOD for sand of 0.27 kg Na2S2O8/
tone (Tsitonaki et al., 2010). Fig. 8 compares the environmental
impacts of two ISCO scenarios applying permanganate (525 tonnes)
and persulfate (300 tonnes) respectively. The persulfate scenario
shows a reduction in global warming, ozone formation, terrestrial
eutrophication and respiratory impacts by 20e40% compared to
the permanganate scenario, mainly due to a lower energy use for
the production of the smaller amount of persulfate. However, at the
same time acidication increases by 80%, the aquatic eutrophication by a factor of 5, and the ecotoxicity and human toxicity by
10e30% (see Fig. 8) due to the high contribution to these impact
categories from persulfate production.
4.2. Primary impacts
The long-term monitoring scenario causes the largest release of
contaminant mass to groundwater over its timeframe (23.2 kg of
TCE), whereas remediation by ERD reduces this to 1.1 kg VC and
400
ISCO (80 y)
Ecotoxicity freshwater
Respiratory inorganics
Aquatic eutrophication
Terrestrial eutrophication
Acidification
Ozone formation (Human)
Global Warming
Human toxicity (cancer)
Human toxicity (non-cancer)
Ecotoxicity freshwater
Respiratory inorganics
Aquatic eutrophication
Terrestrial eutrophication
Acidification
Ozone formation (Human)
Global Warming
0%
10%
20%
30%
40%
50%
60%
70%
80%
90%
Contribution to impacts
Injection wells
Monitoring
Bioculture
Primary impact VC
Activated Carbon
100%
1500 PE
1650 PE
350
401
300
250
200
150
100
50
0
Global
warming
Ozone
f ormation
Acidif ication
Terrestrial
Aquatic
eutrophication eutrophication
ISCO (permanganate)
Respiratory
inorganics
Ecotoxicity
f reshwater
ISCO (persulfate)
Fig. 8. Life cycle comparison of ISCO using permanganate and persulfate as an oxidant.
Long-term monitoring
ERD (high rate)
ERD (low rate)
ISCO
2250 PE
Long-term monitoring
and activated carbon
200
400
600
800
1000
1200
Fig. 9. Comparison of total primary impacts (in PE) and secondary impacts (in PE) of
the ve management options. Note that the normalized impacts are a summation of
the individual impacts, i.e. assuming equal weighting of each impact type.
402
management option, regulatory bodies must accept that the longterm monitoring option causes the groundwater quality criterion
for TCE to be exceeded for 800 years. If long-term monitoring is
combined with activated carbon treatment at the waterworks, this
option will lead to larger secondary environmental impacts than
ERD, but will still be preferable to the ISCO scenario. Finally ERD is
only favorable if it can be ensured that it does not cause any
signicant leaching of VC to the groundwater. If such leaching
occurs, the benets of ERD are lost because even small amounts of
VC result in very high primary toxic impacts.
It should be noted, that the conclusions in this paper are drawn
on the basis of a case study with a clay till site geology resulting in
a long remediation timeframe. In more permeable settings with
faster remediation, other conclusions may be reached. The ndings
from this study show that risk assessment and life cycle assessment
of management options for a contaminated site can be combined to
provide a more holistic assessment and an improved basis for
decisions on the selection of a management strategy for a contaminated site.
Acknowledgments
The work was funded by the Region of Southern Denmark, the
Technical University of Denmark and REMTEC, Innovative REMediation and assessment TEChnologies, Danish Council for Strategic
Research. Mette Christophersen and Jan Petersen (Region of
Southern Denmark), Claus Westergaard (Orbicon), Arkil A/S and
Glibstrup A/S are acknowledged for providing valuable data on the
site and for the LCA.
Appendix A. Suppoting information
Supporting information related to this article can be found at
http://dx.doi.org/10.1016/j.jenvman.2012.08.002.
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