Science of the Total Environment 408 (2010) 4672–4680

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Science of the Total Environment

j o u r n a l h o m e p a g e : w w w. e l s ev i e r. c o m / l o c a t e / s c i t o t e n v

Life-cycle assessment of selected management options for air pollution control

residues from waste incineration
Thilde Fruergaard, Jiri Hyks, Thomas Astrup ⁎
Department of Environmental Engineering, Miljoevej, Building 113, Technical University of Denmark, 2800 Kgs. Lyngby, Denmark

a r t i c l e i n f o a b s t r a c t

Article history: Based on available technology and emission data seven selected management options for air-pollution-
Received 18 February 2010 control (APC) residues from waste incineration were evaluated by life-cycle assessment (LCA) using the
Received in revised form 17 May 2010 EASEWASTE model. Scenarios were evaluated with respect to both non-toxicity impact categories (e.g. global
Accepted 20 May 2010
warming) and toxicity related impact categories (e.g. ecotoxicity and human toxicity). The assessment
addressed treatment and final placement of 1 tonne of APC residue in seven scenarios: 1) direct landfilling
Keywords:
LCA
without treatment (baseline), 2) backfilling in salt mines, 3) neutralization of waste acid, 4) filler material in
Waste incineration asphalt, 5) Ferrox stabilization, 6) vitrification, and 7) melting with automobile shredder residues (ASR). The
Residues management scenarios were selected as examples of the wide range of different technologies available
Air pollution control worldwide while at the same time using realistic technology data. Results from the LCA were discussed with
APC respect to importance of: energy consumption/substitution, material substitution, leaching, air emissions,
Hazardous waste time horizon aspects for the assessment, and transportation distances. The LCA modeling showed that
thermal processes were associated with the highest loads in the non-toxicity categories (energy
consumption), while differences between the remaining alternatives were small and generally considered
insignificant. In the toxicity categories, all treatment/utilization options were significantly better than direct
landfilling without treatment (lower leaching), although the thermal processes had somewhat higher
impacts than the others options (air emissions). Transportation distances did not affect the overall ranking of
the management alternatives.
© 2010 Elsevier B.V. All rights reserved.

1. Introduction primarily rely on local traditions and conditions rather than on a

Residues from municipal solid waste (MSW) incinerators have
received considerable attention within recent decades and numerous
studies have been carried out focusing on treatment, utilization, and
leaching mechanisms (e.g. Kirby and Rimstidt, 1994; Kosson et al.,
2002; Dijkstra et al., 2008). While bottom ashes can serve as excellent
construction materials after simple treatment (Van Gerven et al.,
2005; Astrup, 2007), air pollution control (APC) residues are
categorized as hazardous waste and are generally not suited for
utilization due to their poor technical properties and high contents of
salts and heavy metals (Hjelmar, 1996; Hyks et al., 2009a). Over the
years significant efforts have been placed on developing stabilization
processes focusing on immobilizing heavy metals in APC residues
(Kinto, 1996; Iretskaya et al., 1999; Ecke et al., 2000; Lundtorp et al.,
2002; Cai et al., 2003; Aguiar del Toro et al., 2009) and while
numerous processes have been implemented worldwide, no specific
trend has emerged with respect to the stabilization approach (Astrup,
2008). Apparently, management strategies and selection of processes
⁎ Corresponding author. Tel.: + 45 4525 1558; fax: + 45 4593 2850.
E-mail address: tha@env.dtu.dk (T. Astrup).
systematic evaluation of environmental benefits and drawbacks.
Today APC residue management strategies can be categorized by
the following process types (Chandler et al., 1997; Sabbas et al., 2003;
Astrup, 2008): i) extraction and separation, ii) chemical immobiliza-
tion, iii) solidification, and iv) thermal treatment. While the simpler
processes, such as extraction, solidification and to some extent
chemical immobilization, only require limited use of resources
(energy and materials) they may also provide less-than-perfect
stabilization. Thermal treatment on the other hand may potentially
provide excellent stabilization but also use substantial energy in the
process. Ideally, when selecting a specific treatment process stake-
holders should balance such aspects accounting for relevant indirect
consequences too. This is, however, a complicated task and is done
only in very rare occasions.
With numerous processes available worldwide (Astrup, 2008)
selecting the best treatment and disposal options for APC residues
from an environmental point of view may not be an easy task. To
provide an improved basis for waste incinerators and approving
authorities, coherent evaluations of benefits and drawbacks related to
the wide range of treatment and disposal options available are
necessary. Life-cycle assessment (LCA) is a suitable method for such
an evaluation as it provides a holistic approach by aiming at including

0048-9697/$ – see front matter © 2010 Elsevier B.V. All rights reserved.
doi:10.1016/j.scitotenv.2010.05.029
 T. Fruergaard et al. / Science of the Total Environment 408 (2010) 4672–4680
and quantifying all direct and indirect emissions and resource
consumptions throughout the life-cycle of the considered system.
During the past 15–20 years life-cycle assessment has been a widely
applied tool for assessment of waste management solutions, but only
a few studies have focused on the environmental aspects of ash
management. Olsson et al. (2006), Birgisdóttir et al. (2007) and
Carpenter et al. (2007) focused on utilization of bottom ashes from
waste incineration, whereas Mroueh et al. (2001) and Babbitt and
Lindner (2008a,b) evaluated the environmental impacts of utilization
of fly ashes from coal combustion. Toller et al. (2009) focused on two
ash types: MSW bottom ash and wood fly ash. No studies on
environmental assessments of APC residues were found.
The overall aim of this paper was to compare seven selected
treatment and disposal options for APC residues in a life-cycle
perspective representing a wide range of process types used around
the world. With these processes as examples and based on actual data
collected for both full-scale and pilot-scale installations, the paper i)
quantifies the potential environmental impacts and highlights
significant emissions from the selected alternatives, ii) evaluates
critical boundary conditions and uncertainties, and iii) provides
important recommendations for future management of these residues.
2. Modeling approach
2.1. Life-cycle assessment framework
The functional unit was “treatment and final disposal of one tonne
of APC residue, including secondary and avoided processes”. The time
horizon of the LCA was 100 years, focusing on environmental impacts
within a foreseeable future. The impacts of this choice were discussed
in Section 4.4. To provide more generic conclusions, an average
chemical composition of APC residues from a range of Danish
incinerators with semi-dry and wet flue gas cleaning systems was
used as a basis for the assessment. The importance of this choice was
discussed in Section 4.3.
The assessment included consumption of energy and resources
for managing residues, emissions to air/water/soil, secondary
processes (i.e. processing of materials for utilization) and avoided
processes (i.e. avoided production of primary materials substituted
by the residues). Residue transport was assessed separately based
on Danish conditions.
Table 1
Management scenarios assessed in the LCA.
Scenario Description
1 Landfilling without any pretreatment
2a, 2b Utilization as backfilling material
in German salt mines
3a, 3b Utilization for neutralization of waste
acid in Norway
4a, 4b Utilization as filler material in asphalt in the
Netherlands
5 Ferrox stabilization followed by landfilling Water extraction and
chemical stabilization
6 Vitrification followed by landfilling Melting
7a, 7b Thermal co-treatment of APC residues with automobile Melting
shredder waste followed by reutilization and landfilling
4673
Construction and decommissioning of infrastructure, buildings,
machinery, etc. and household-like waste generated in small amounts
from the treatment plants were excluded from the assessment. Their
impacts were assumed to be of similar size for each treatment option
thereby counterbalancing each other out when comparing the
different options. It was considered reasonable to exclude these
impacts as the overall aim of the paper was to compare different
treatment alternatives rather than quantifying the total environmen-
tal impacts of each option.
2.2. Impact assessment: scenarios
The LCA model EASEWASTE (Kirkeby et al., 2006) was used for the
environmental assessment. EASEWASTE is specifically made for LCA
of waste management systems and facilitates a comprehensive
environmental impact assessment by calculating waste flows,
resource consumption and environmental emissions from individual
waste technologies within the system. The model allows flexible
definition of individual scenarios and includes default background
data needed for the assessments of waste systems. The environmental
impacts assessed in this paper followed the EDIP97 methodology
(Wenzel et al., 1997) using the latest version of the normalization
references (Stranddorf et al., 2005). The impact categories included
were: Global Warming (GW), Acidification (AC), Nutrient Enrichment
(NE), Photochemical Ozone Formation (POF), Human Toxicity via Air
(HTa), via water (HTw) and via soil (HTs), and Ecotoxicity in Water
(chronic) (ETw) and in soil (ETs). For Global Warming the scale is
global, for all other categories the results apply to Europe.
Seven overall scenarios were discussed, see Table 1. Each scenario
is briefly outlined below. For technical details regarding the individual
processes, please refer to Astrup (2008).
2.2.1. Scenario 1: landfilling without pretreatment
Scenario 1 involved direct landfilling of the residues without
pretreatment and served as a reference for the discussions in this
paper rather than being a realistic option for residue management in
Denmark. The scenario included average energy consumption for low-
organic landfills (Manfredi and Christensen, 2009), treatment of
collected leachate, and leaching of heavy metals to water and soil
during the 100 year time horizon. The leaching data were based on
Process Material Emissions from
utilization landfill
Leaching from landfill
Solidification in cement a: No substitution No
b: Substitution of
natural aggregates
Water and acid a: No substitution No, but wastewater emissions
extraction, solidification b: Substitution of
in gypsum limestone
Solidification in asphalt Substitution of a: Leaching from
limestone solidified material based on lowest data values in
Scenario 5 and 6
b: Leaching from solidified material based on highest
data values in Scenario 5 and 6
Wastewater emissions and leaching from landfill
Leaching from landfill
Substitution of energy Leaching from solidified material
and natural aggregates
a: Avoids landfilling of
shredder waste
b: Avoids incineration
of shredder waste
4674 T. Fruergaard et al. / Science of the Total Environment 408 (2010) 4672–4680
field-scale lysimeters with two Danish APC residues (DTU et al., 2001;
Hyks et al., 2009b).
2.2.2. Scenario 2: backfilling in salt mines
Scenario 2 represented a commonly used management option
with backfilling of salt mines in Germany. The scenario included
energy consumption for mixing the residues with water, additives and
other materials (often other waste/residual materials), and pumping
the cement-like slurry into the salt mines to avoid potential collapse
of the mines. Based on Astrup (2008), two alternatives were
addressed. In the first alternative (Scenario 2a) no material substitu-
tion was expected to occur based on the assumption that the residues
substitute other waste materials also utilized in the mines rather than
natural aggregates like sand, gravel or soil. In the second alternative
(Scenario 2b) 1 tonne of APC residues was assumed to substitute
1 tonne of natural aggregates. In both cases, no leaching from the
disposed residues was assumed due to the limited hydraulic contact
between host rock (salt) formations and the surrounding groundwa-
ter bodies (European Commission, 2003).
2.2.3. Scenario 3: neutralization of waste acids
Scenario 3 represented a Norwegian technique in which APC
residues were mixed with water and waste acid from the titanium
industry, thereby utilizing the residues for neutralization of the waste
acid. The treated residues were subsequently (in the form of a gypsum
containing slurry) used for reconstruction of an old limestone quarry.
Energy consumption for mixing the residues and pumping the slurry
was included. Similarly to Scenario 2, two alternatives were modeled
assuming either no material substitution as limestone was available
on-site (Scenario 3a), or avoided production of 35 kg limestone per
tonne of APC residues (Scenario 3b) otherwise needed for neutral-
izing the waste acid. Similarly to Scenario 2, leaching from the
disposed residues to the surrounding aquifer was not considered
relevant as the site was not hydraulically connected with the recipient
(Astrup, 2008). However, excess process water at the site was
discharged to the sea after treatment (heavy metals emissions in
the treated process water were included in the LCA).
2.2.4. Scenario 4: filler material in asphalt
Scenario 4 represented use of APC residues as filler material for
asphalt production: 1 tonne of limestone was assumed substituted
(Astrup, 2008). Energy for grinding and mixing the APC residues
during asphalt production was assumed identical to the energy
demand for grinding and mixing the limestone with the other
materials in the filler and therefore excluded from the assessment.
Leaching data for APC residues used as filler in asphalt was not
available; however, in agreement with data from Chandler et al.
(1997) and Vondruska et al. (2002) it was assumed that leaching from
the “asphalt stabilized” residues was higher than from vitrified
materials (see Section 2.2.6) but lower than from Ferrox stabilized
residues (see Section 2.2.5). The two levels of leaching were
addressed in separate alternatives: Scenario 4a and 4b, respectively.
2.2.5. Scenario 5: Ferrox stabilization followed by landfilling
Scenario 5 represented a chemical stabilization technique in which
the APC residues were mixed with water and FeSO4·7H2O followed by
aeration and chemically binding of heavy metals (Lundtorp et al.,
2002). Removal of soluble salts reduced the weight of the APC residues
to 860 kg. The stabilized residues were assumed landfilled similar to
Scenario 1. FeSO4·7H2O is a by-product from the titanium industry and
no environmental costs was associated with its production. Only
transportation of FeSO4·7H2O (80 kg per tonne of APC residues
transported 500 km by boat) was considered. Energy consumption
for the stabilization and treatment of process water as well as heavy
metal emissions in the process water were included (DTU et al., 2001).
The leaching data were obtained from field-scale lysimeters on two
different Ferrox-treated APC residues (DTU et al., 2001).
2.2.6. Scenario 6: vitrification followed by landfilling
Scenario 6 represented a generic thermal treatment process in
which residues were vitrified. The scenario included energy con-
sumption for the thermal process as well as air emissions (Astrup,
2008). The vitrification process reduced the weight of the APC
residues to 800 kg but generated 60 kg of new APC residues (a range
of metals are transferred to the off-gas during thermal treatment and
the gas needs cleaning). The stabilized residues were landfilled similar
to Scenario 1. Leaching from the treated residues was estimated based
on literature values (Nishigaki, 1996; Kinto, 1996; Jimbo, 1996; Sakai
and Hiraoka, 2000; Sung et al., 2005; Rani et al., 2008; Andreola et al.,
2008) while accounting for typical “leaching control” from such ashes
(Kosson et al., 2002; van der Sloot et al., 2001; Hyks et al., 2007,
2009a; Dijkstra et al., 2008). The newly formed APC residues cannot
be landfilled directly but needs stabilization/pretreatment. In this
paper, management of these new residues was assumed done
similarly to Scenario 3b for simplicity reasons.
2.2.7. Scenario 7: thermal co-treatment with automobile shredder
residue (ASR) followed by reutilization and landfilling
Co-treatment with ASR has been considered as management
option in Denmark and Switzerland (Astrup, 2008). Scenario 7
represented a process in which 1 tonne of APC residues was thermally
treated with 1 tonne of ASR. As such this process is similar to
vitrification, except that part of the energy used in the melting process
is supplied by the ASR. ASR was in this case assumed to have a particle
size below 12 mm and a lower heating value of about 7.6 GJ/tonne
(based on tests by Elsam, 2006), indicating that only a part of typical
ASR was considered. Consumption of energy and auxiliary materials
(oxygen, natural gas and CaCO3), air emissions from the melting
process, emissions of heavy metals from the wastewater treatment
plant and substitution of energy due to the heating value of ASR
(Table 3) were included. The process created bottom ash, sludge,
gypsum and new APC residues. The bottom ash (1.4 tonne) was
assumed to substitute natural aggregates in road construction with a
lifetime of 100 years. Utilization in road construction can be expected
to generate leaching of heavy metals (Aberg et al., 2006; Birgisdóttir
et al., 2007), which were assumed to be distributed by 15% to surface
water and 85% to soil. Sludge, gypsum and new APC residues (in total
400 kg) were assumed to be treated similar to the residues in Scenario
3b for simplicity reasons.
Two alternatives were modeled for the avoided management of
ASR: avoided landfilling of ASR in Scenario 7a (current practice in
Denmark), and avoided incineration of ASR in Scenario 7b (currently
discussed in Denmark). In the first alternative, energy consumption at
the landfill and leaching of heavy metals were avoided and therefore
subtracted from the results. In the second alternative, air emissions
and energy recovery associated with ASR incineration was subtracted
(it was assumed that the avoided electricity and heat generation from
ASR incineration was identical to the electricity and heat generation
obtained during co-treatment with APC residues; consequently no net
energy substitution was assumed for Scenario 7b).
2.3. Common boundary conditions for all scenarios
In all scenarios, residues landfills were assumed located in a coastal
area minimizing the environmental impacts from leached salts. All
landfills were assumed being 10 m high with a bulk density of the
landfilled material of 1 tonne/m3. During the first two years a yearly
leachate generation corresponding to a net infiltration of 500 mm was
assumed, and thereafter a top cover was assumed established reducing
the leachate generation considerably.
 T. Fruergaard et al. / Science of the Total Environment 408 (2010) 4672–4680 4675

Leachate collection was assumed active throughout the entire 100-
year time period of the assessment; however, a worst case situation
was considered assuming a progressive deterioration of the bottom
liner performance. This resulted in decreasing leachate collection
efficiency over time: from 95% efficiency during the first 20 years to
60% the last 25 years. The first 50 years all collected leachate was
assumed to be treated at a wastewater treatment plant (WWTP), in
the latter period all collected leachate was assumed to be discharged
directly to the sea. Sludge from the WWTP (containing the removed
heavy metals) was assumed distributed at fields and the heavy metals
accordingly ending up as soil emissions. The WWTP was not assumed
to be 100% efficient and specific heavy metals removal efficiencies
were applied in the WWTP based on Manfredi and Christensen
(2009). The heavy metals not removed at the WWTP were assumed
discharged to surface waters, whereas heavy metals in the non-
collected leachate ended up in the groundwater (Manfredi and
Christensen, 2009).
Air emissions from the specific thermal treatment processes
(Scenarios 6 and 7) were not available but were instead estimated
based on element transfer coefficients for typical waste incinerators
(i.e. fractions of an element in the input emitted to air, see Riber et al.,
2008). The solid composition of the APC residues as shown in Table 2
was used as input. In Scenario 7, the residues were co-treated with
automobile shredder residues and the transfer coefficients were
applied to this mixture. The transfer coefficients were within the
range 0–0.35 corresponding to incineration in a modern MSW
incinerator (Riber et al., 2008; Pedersen et al., 2009).
Electricity and heat consumed or substituted within the
scenarios were assumed to be produced at combined heat and
power plants using coal as fuel. Assumptions regarding energy may
potentially be important; however the choice of coal as fuel for
energy production follows common practice within LCA (for
further details, refer to Fruergaard et al., 2009). The emissions
and fuel consumptions at these plants were typical for Danish
conditions and allocated based on energy quality, i.e. based on an
assumption that electricity has a higher quality than heat and
thereby associated with a relatively larger share of the emissions
and fuel consumption (Fruergaard et al., 2009). The environmental
load of electricity generation was thereby approximately six times
higher than heat generation. Energy and resource consumption/
substitution is summarized in Table 3.
3. Results
The potential environmental impacts of the considered manage-
ment alternatives are shown in Fig. 1 as normalized impact potentials
in milli-person equivalents (mPE). 1 PE represents the annual impacts
from an average person in a given area. Positive values correspond to
environmental loads while negative values represent savings. The
environmental impacts were divided into two groups, the energy
related impacts (non-toxic impacts) and the toxic, shown in the upper
and lower part of Fig. 1, respectively. A summary of the main impacts
is provided in Table 4.
The largest impact potentials within the non-toxic impacts were
associated with Global Warming (GW), Acidification (AC) and
Nutrient Enrichment (NE). These three impact categories are all
highly related to energy consumption and thus the trends applicable
for GW generally also apply for AC and NE. Consequently, a treatment
alternative with a large GW potential will usually also contribute with
relatively large AC and NE potentials: in the following text, only GW is
therefore discussed.
In the toxic impact categories, the most important impact
potentials were related to Ecotoxicity in Water (chronic) (ETw), and
Human Toxicity via water (HTw) and via soil (HTs). The impact
potentials of Ecotoxicity in Soil (ETs) and Human Toxicity via air
(HTa) were insignificant and are thus omitted from the figures. It
should be noted that the two impact groups are not directly
comparable: generally the toxic impacts are considered more
uncertain than the non-toxic impact categories (Finnveden et al.,
2009). This does not indicate that these impacts are not relevant, only
that lack of inventory data and lack of consensus concerning the

Table 2
The bulk contents of elements considered in the LCA shown together with corresponding emissions for 100 years of leaching.

Total content (mg/kg TS) Cumulated leaching emissions in evaluated treatment scenarios (mg/kg TS)

Element This Literatureb Scenario Scenario Scenario Scenario Scenario Scenario Scenario
studya 1c 2 3 5c 6f 7g
4ae 4be

Al 27 × 103 10–81 × 103 2.72 0 0 1.85 1.91 1.91 1.85 1.85h

As 260 10–380 0.03 0 0 0.07 0.08 0.08 0.07 0.02
Cd 340 100–796 0.03 0 0 0.002 0.004 0.004 0.002 0.0003
Cl 130 × 103 40–220 × 103 50.4 × 103 0 0 20 15.8 × 103 15.8 × 103 20 3.2
Co 52 6–69 0.008 0 0 0.004 0.008 0.008 0.004 0.004h
Cr 450 12–840 0.07 0 0 0.45 1.71 1.71 0.45 0.03
Cu 1.4 × 103 0.3–1.3 × 103 0.04 0 0 0.02 0.13 0.02 0.13 0.007
Fe 13 × 103 3–63 × 103 1.05 0 0 0.11 1.1 0.11 1.1 1.1h
Hg 25 0.4–55 0.002d 0 0 0.002 0.005 0.005 0.002 0.0001
Mn 740 0.3–1.6 × 103 0.02 0 0 0.02 0.08 0.08 0.02 0.002
Mo 35 2–37 0.62 0 0 0.004 6.25 6.25 0.004 0.004h
Ni 61 15–110 0.005 0 0 0.007 0.02 0.007 0.02 0.003
Pb 5.7 × 103 1.5–17.1 × 103 65.7 0 0 0.004 1.68 0.004 1.68 0.002
Sb 820 0.2–3.2 × 103 0.05 0 0 0.02 0.14 0.14 0.02 0.02h
Zn 32.6 × 103 4–38 × 103 1.32 0 0 0.46 0.59 0.59 0.46 0.02

Values shown in italic indicate that lower than detection limit data were found at several occasions during literature research.
a
Average chemical composition of APC residues from a range of Danish incinerators with either semi-dry or wet flue gas cleaning systems (DTU et al., 2001; Hyks et al., 2007).
b
Typically observed in APC residues (Bodog et al., 1996; Chandler et al., 1997; Lundtorp et al., 2002; Youcai et al., 2002; Li et al., 2004; Yang et al., 2008; Rani et al., 2008;
Hyks et al., 2009a).
c
Numerical integration of lysimeter leaching curves (DTU et al., 2001; Hyks et al., 2009b).
d
Hjelmar (1996).
e
Leaching data from Scenario 5 and 6 are applied in Scenario 4a,b as boundaries; see Section 2.2.4 for details.
f
Maximum estimated leaching after recalculating leaching data from L/S 10 leaching experiments (Nishigaki, 1996; Kinto, 1996; Jimbo, 1996; Sakai and Hiraoka, 2000; Rani et al.,
2008; Andreola et al., 2008).
g
Elsam (2006).
h
Due to lack of specific data, values from Scenario 6 were used assuming similar physical-chemical properties.
4676 T. Fruergaard et al. / Science of the Total Environment 408 (2010) 4672–4680

Table 3
Material and energy flows per tonne of APC residue.

Scenario Description Energy use/tonne of residue Substitutions

1 Landfilling without any pretreatment Activities on landfill: 2.5 l diesel

2 kWh el
Leachate treatment: 4 kWh el
2a + b Utilization as backfilling material in German salt mines Mixing and pumping: 1.5 l diesel a: No substitution
29 kWh el b: 1 t of natural aggregates
3a + b Utilization for neutralization of waste acid in Norway Washing and pumping: 0.6 l diesel a: No substitution
13 kWh el b: 35 kg limestone
4 Utilization as filler material in asphalt in the Netherlands 1 t of limestone
5 Ferrox stabilization followed by landfilling Stabilization process: 34 kWh el
0.6 l diesel
Landfilling of residue (0.86 t): 2.5 l diesel
2 kWh el
Leachate treatment (0.86 t): 4 kWh el
6 Vitrification followed by landfilling Melting process: 700 kWh el
Landfilling of residue (0.8 t): 2.5 l diesel
2 kWh el
Leachate treatment (0.8 t): 4 kWh el
Landfilling of new APC (0.06 t): Similar to Scenario 3b
7a + b Thermal co-treatment of APC residues with automobile Melting process: 210 kWh el a: 550 kWh el
shredder waste followed by reutilization and landfilling 76 kg natural gas a: 1350 kWh heat
697 kg oxygen a + b: 1.4 t of natural aggregates
Landfilling of new APC (0.4 kg): Similar to Scenario 3b

characterization method used have resulted in these impacts being

considered less robust than the non-toxic impacts.

3.1. Global warming (GW)

Vitrification (Scenario 6) showed the largest GW potential due to

the large energy consumption, see Table 3. Also the thermal co-
treatment process (Scenario 7) contributed significantly to GW,
especially when incineration was the alternative option for ASR
(Scenario 7b). Avoiding incineration of ASR resulted in a loss of energy
production within the system (i.e. the same amount of energy needed
to be produced elsewhere). No net energy substitution was therefore
occurring in Scenario 7b. The net contribution to GW came from
production of the relatively large quantity of O2 (697 kg O2/tonne APC
residues) used in the thermal process. In the process, carbon in the
ASR is converted into CO2 which also contributed to GW; however,
this contribution was out-balanced by an identical CO2 emission from
ASR incineration.
When landfilling was considered the alternative management
option for ASR, the GW potential of Scenario 7a (avoiding landfilling
of ASR) was only half of that in Scenario 7b. In Scenario 7a the net energy
production was positive because the energy content of ASR was not
assumed utilized when ASR was landfilled (i.e. a benefit as energy is
substituted elsewhere). However, landfilling saves potential CO2
emissions by storage of the carbon content in the ASR (i.e. a benefit
compared with the thermal processes). Overall, the GW potential of
Scenario 7a would have been negative (causing an environmental
saving) without the large O2 consumption in the thermal co-treatment
process. Everything considered the GW potential for the scenario
consequently is positive, representing a load.
In the remaining scenarios the GW potential is only of minor
importance, because of very low energy consumptions (Table 3).

3.2. Ecotoxicity in water (ETw)

The largest environmental load with respect to ETw (Fig. 1) was

Fig. 1. Environmental impacts from treatment of one tonne of APC residue in milli-
person equivalents (mPE). Transportation of the residues is not included.
observed for landfilling without pretreatment (Scenario 1). This was
caused by emissions of Pb from the landfilled residues (97% of the
total impact potential). Ferrox stabilization (Scenario 5) and vitrifi-
cation (Scenario 6) also contributed to ETw, although much less than
Scenario 1.
 T. Fruergaard et al. / Science of the Total Environment 408 (2010) 4672–4680 4677

Table 4
Affected impact categories, scenarios with highest impacts, significant activities and emissions.

Impact category Scenarios contributing Significant activities Significant emissions

Global warming (GW) 6 Energy consumption — melting process CO2

7b Energy consumption — melting process CO2
7a Energy consumption — melting process CO2
Ecotoxicity in water (ETw) 1 Leaching from landfill Pb
5 Wastewater from stabilization process Mo in wastewater
Leaching from landfill Mo in leachate from landfill
6 Energy consumption — melting process PAH and Sr
Leaching from landfill Cu, Cd, Pb
Human toxicity via water (HTw) 1 Leaching from landfill Pb
6 Air emissions from melting process Hg
7a + 7b Air emissions from melting process Hg
Human toxicity via soil (HTs) 6 Air emissions from melting process Sb, Hg, As
4b Emissions to soil from filler material Mo, Sb, Cr
1 Leaching from landfill Pb, Sb, As
5 Wastewater from stabilization process Mo in wastewater
Leaching from landfill Mo and Cr in leachate from landfill
7a + 7b Air emissions from melting process As, Hg, Cr

Around 40% of the total impact potential related to the Ferrox
stabilization was caused by the stabilization process itself (mainly
emissions through wastewater) while the remaining impacts were
associated with leaching from the landfilled residues after stabiliza-
tion. Mo constituted the largest contribution, both in case of
wastewater and leachate.
Contrary to Ferrox stabilization, numerous activities contributed to
ETw in case of vitrification. The most important were the electricity
consumption for heating the residues (40% of total, important
emissions were poly-aromatic hydrocarbons (PAHs) and Sr), air
emissions from the thermal treatment process (16% of total,
important emissions were Cd, Hg, Pb and Cu), leaching from landfilled
residues after treatment (29% of total, important emissions were Cu,
Cd and Pb), and production of diesel oil for the trucks used at the
landfill (12% of total, important emissions were PAH and Sr). Energy
related emissions of PAH and Sr were associated with fuel combustion
(PAH) and provision of the fuel (Sr), note in this context that the Sr
emissions can be considered rather uncertain and both PAH and Sr
emissions should be interpreted with caution.
3.3. Human toxicity via water (HTw)
Similar to ETw this impact category was dominated by landfilling
of non-treated residues (Scenario 1). Here emissions of Pb from the
landfilled residues accounted for 99% of the total impact potential. The
majority of impacts related to the thermal processes (Scenario 6, 7a
and 7b) were caused by emissions of Hg to air generated when the
residues were thermally treated.
3.4. Human toxicity via soil (HTs)
The last toxicity category affected by the investigated treatment
alternatives was HTs. No treatment option dominated this category;
however, the largest contribution was observed for vitrification
(Scenario 6). The majority of the impacts in Scenario 6 were caused
by air emissions of especially Sb, Hg and As associated with the
thermal process. The impact potentials related to utilization of
residues in asphalt (Scenario 4b) and direct landfilling (Scenario 1)
were of almost equal size, although smaller than for vitrification. The
impacts from Scenario 4b were exclusively caused by emissions to soil
from the residues used as filler material: especially Mo, but also Sb
and Cr. In Scenario 1 the impacts were caused mainly by emissions to
soil from the landfilled residues: especially emissions of Pb, but also
smaller contributions from Sb and As.
Ferrox stabilization (Scenario 5) and thermal co-treatment with ASR
(Scenarios 7a and 7b) also had relatively small contributions to HTs. As
was the case for ETw, contributions in Scenario 5 were divided between
the wastewater and leaching from the landfilled residues. Especially Mo
emissions to soil caused a significant impact from both the wastewater
(80% of overall impact in this category) and the landfilled materials (65%
of overall impact). Cr and Sb in the leachate from the landfilled residues
also appeared to contribute significantly to HTs. The impacts in
Scenarios 7a and 7b were caused mainly by air emissions from the
melting process, especially As and to a minor degree Hg and Cr.
4. Discussion
4.1. Which is the best management strategy?
As can be realized from the results outlined above and Table 4, two
types of impacts were associated with the residue management
alternatives: those related to Global Warming and those related to the
toxicity categories. GW impacts were generally related to energy
consumption while toxicity impacts were generally related to either
air emissions or leaching. Consequently, management alternatives
consuming little energy and at the same time generating low
emissions of metals would turn out as best. Such an alternative
may; however, not be available. Direct landfilling had the highest
environmental loads in the ETw and HTw categories, while the
vitrification alternative had the highest environmental load with
regard to GW and also relatively high loads regarding HTw and HTs.
The scenarios with the lowest environmental loads in most categories
were utilization as backfilling material in salt mines, utilization for
neutralization of waste acid, and (when low emission levels were
assumed) utilization as filler material in asphalt. This was due to very
low energy consumptions in the treating processes and subsequently
no or very low emissions from the disposed residues.
Based on the results discussed above, the preferable management
alternatives were utilization as backfilling material in salt mines,
utilization for neutralization of waste acid, and utilization as filler
material in asphalt. The least preferable option were landfilling
without pretreatment and vitrification followed by landfilling. The
most important emissions were CO2, Hg, Sb, As and Cr to air, and Pb,
Mo, Cu, Cd, As and Cr to water and soil.
4.2. Importance of residue transportation
Transportation of residues was excluded from the results dis-
cussed previously; however, to better illustrate the importance of
transportation distances, the situation for transport of Danish residues
was discussed in the following. Scenarios 2–4 typically require longer
transportation distances as these are currently only offered in
4678 T. Fruergaard et al. / Science of the Total Environment 408 (2010) 4672–4680
Fig. 2. Environmental impacts from treatment of one tonne of APC residue in milli-
person equivalents (mPE). Transportation of the residues is included.
Germany, Norway and the Netherlands, respectively. The remaining
scenarios have been assumed to take place in Denmark. The following
transport distances and transportation means were assumed: 100 km
by truck (Scenario 1, 5–7), 700 km by truck (Scenario 2, 4), 300 km by
truck + 300 km by ship (Scenario 3). The modeling results including
transportation are shown in Fig. 2.
Generally, transportation appeared to affect most impact catego-
ries due to the multiple substances emitted from fuel combustion. For
the non-toxic categories especially GW was affected by CO2 emissions,
but also AC, NE and POF were affected to a minor degree. AC was
typically affected by emissions of SO2 and NOx, NE due to NOx
emissions and POF due to emissions of non-methane volatile organic
compounds (NMVOCs) and volatile organic compounds (VOCs). For
the toxicity categories especially ETw was affected mainly by
emissions of PAHs.
Including transportation did not change the overall ranking with
respect to the least preferred option; however, identifying the best
option became less clear (see Fig. 2). The reason for this was that
scenarios having the lowest environmental impacts without trans-
portation also had the longest transport distances needed. The
differences between Scenarios 1–5 when including transportation
was for most impact categories insignificant. Overall, transport
distances significantly affected the LCA result for management options
with little energy consumption in the treatment process, while
transport appeared less important in case of processes involving
considerable energy consumption such as thermal processes.
4.3. Sensitivity assessment of the results
An integral part of performing an LCA is to assess the sensitivity of
the results towards changes in the assumptions. For the scenarios
discussed in this paper the main uncertainties are considered to be
related to: 1) energy consumption and substitution, 2) material
substitution, 3) leaching from landfilled residues, and 4) air emissions
from thermal treatment processes. The largest uncertainties were
likely related to 3) and 4) as these data were partly estimated based
on literature values. The importance of these assumptions for the
conclusions is discussed in the following.
4.3.1. Energy consumption and substitution
As previously discussed, energy consumption in the thermal
treatment processes significantly contributed to the impacts in the
non-toxicity categories for these scenarios. Electricity used in the
treatment processes was assumed to be produced from coal, and to
test the importance of this assumption, modeling with natural gas,
which is generally considered as a relatively clean fuel was also
carried out. All four non-toxicity categories (especially GW) were
affected whereas the toxicity categories were almost unaffected. The
GW potential for vitrification (Scenario 6) was reduced to half of the
original size due to natural gas being a less CO2-intensive fuel than
coal. The GW potential for the melting process (Scenario 7a) was
increased by a factor 4 as the energy produced from the ASR now
substituted a less CO2-intensive fuel rather than coal. The GW
potential in Scenario 7b remained the same as ASR was here assumed
incinerated (thereby also producing energy) if not co-treated with the
residues.
Although assumptions regarding fuels for energy significantly
affected the results quantitatively, still the thermal processes had
significantly higher impacts in the non-toxicity categories than the
other management alternatives. Therefore assumptions regarding fuel
types did not affect the overall conclusions of the LCA.
4.3.2. Material substitution
The extent of material substitution when utilizing the residues for
backfilling in salt mines (Scenario 2) and neutralization of waste acids
(Scenario 3) may be relatively uncertain as little information could be
found in this regard. To assess the importance of this assumption, two
alternatives of these scenarios were modeled: with and without
substitution of virgin materials (natural aggregates and limestone,
respectively). In both cases substitution had no significant effect on
the impact potentials. For utilization of residues in asphalt production
(Scenario 4) impacts related to substitution of limestone were
insignificant relative to those from leaching and thereby of minor
importance. Similar in case of the melting process (Scenario 7) in
which bottom ashes generated in the process were assumed utilized
for road construction; again impacts related to substitution of natural
aggregates appeared insignificant compared with the other impacts
from the process.
Overall, assumptions regarding material substitution did not
appear to affect the overall conclusions of the LCA.
4.3.3. Leaching from landfilled residues
Although leaching experiments generally provide robust data for
incineration residues, using leaching data from various sources in an
LCA should always include an evaluation of potential uncertainties
(Hyks et al., 2007, 2009c; Wehrer and Totsche, 2008). Metal leaching
from incineration residues is generally controlled by the geochemical
conditions in the leaching system rather than the metal content in the
 T. Fruergaard et al. / Science of the Total Environment 408 (2010) 4672–4680
solid phase. Typically, less than a few percent of the solid contents are
released by leaching (Astrup et al., 2006a,b). It is therefore considered
unlikely that the residue composition used in this LCA could
significantly affect the conclusions.
No leaching was assumed to occur in Scenario 2 and 3 and these
scenarios are not discussed any further. Field scale leaching data were
available only for Scenario 1, 5, and 7, but some of the elements in
Scenario 1 and especially Scenario 7 had to be estimated based on
literature data (see Table 2). The missing elements were all
comparable with literature values for similar processes and the
associated leaching showed no significant contribution to the overall
impacts.
No data were available for leaching in Scenario 4 (utilization of
APC residues in asphalt), and leaching was instead estimated based on
specific knowledge concerning leaching from asphalt. Two levels of
leaching was modeled to assess the importance of these assumptions.
Only one impact category (HTs) was significantly affected by the
choice of leaching data, mainly caused by emissions of Mo when
leaching was assumed at the highest level. It is; however, considered
more likely that real leaching would be lower and therefore that the
importance of uncertainties on leaching in this case is minor.
For Scenario 6 (vitrification) leaching was based on a vast number
of studies, and the results were accordingly considered robust.
Overall, even though leaching was significant for some scenarios,
the results of the LCA showed to be robust with respect to the
assumptions made regarding missing data. The overall ranking
between the individual scenarios was not affected as the results
were influenced by other factors than leaching.
4.3.4. Air emissions
Air emissions from thermal treatment of residues (Scenario 6 and
7) had significant impacts on the toxicity categories: HTw and HTs. For
HTw the contributions were almost exclusively caused by Hg
emissions. For HTs, Hg was less important, instead Sb and As
contributed considerably. The transfer coefficients for these air
emissions were: 0.20% (As), 0.35% (Hg) and 0.067% (Sb). If actual air
emissions were higher than these levels this would not alter the
overall conclusions of the LCA, but rather worsen the already bad
results for the thermal treatment processes. If, on the other hand,
actual emissions were lower, the thermal treatment processes could
perhaps compete with some of the other processes in the toxicity
categories. As air emissions were calculated based on transfer
coefficients, these emissions were indirectly related to the residue
composition used. As may be realized from Table 2, solid contents of
As, Hg, and Sb were well within typical values for APC residues. It
should however be realized that residue composition vary between
individual incinerators which may potentially affect air emissions
from thermal treatment in some cases.
This indicates that air emissions from thermal processes may be
critical for impacts in the toxicity categories; however, this would not
affect the conclusions with respect to the non-toxicity impacts such as
GW.
4.4. Beyond 100 years: time horizon aspects
A specific challenge for environmental assessment of residue
management is to address potential long-term emissions from disposed
residues as leaching from APC residues may continue potentially for
thousands of years (Astrup et al., 2006a). This LCA covered only a
100 years time horizon illustrating the dilemma either of elaborate
residue treatment today (with energy/recourse consumption and
emissions now) for minimization of future emissions or minimum
handling now with the potential for higher future emissions.
Releases of especially Pb and Mo were high from the non-treated
residues (Scenario 1) significantly affecting ETw and HTw. This
signifies the necessity of subjecting residues to some kind of
4679
treatment. However, the results of the LCA also indicated that the
benefits of treating the residues extensively thereby reducing the
direct leaching can be out-balanced by the indirect emissions from
high energy consumption and generation of new air emissions (as
seen in the thermal treatment processes). The recommendations
based on this LCA are to design treatment processes with low energy
demands and focus utilization of the residues in applications with
minimum leaching. Of the studied scenarios, Scenario 2 (salt mines), 3
(acid neutralization), and 4 (asphalt) fitted best these criteria.
Utilization in salt mines and for neutralization of waste acids
warrants special attention as both options are claimed as having no
long-term leaching. This conclusion is likely based on an assumption
of geological stability in the area, which may be questionable in all
future. In all scenarios; however, only less than 1% of the solid metal
content in the residues were released within the 100 years
corresponding to about L/S 2 l/kg in a leaching test (Hjelmar, 1996;
Hyks et al., 2009a).
No clear consensus currently exists as how to evaluate long-term
impacts within LCA (e.g. Hauschild et al., 2008; Pettersen and
Hertwich, 2008). One approach is to include leaching until concen-
trations reach the background level (Birgisdóttir, 2005). Another
approach is to consider all substances left in the residues after the
100 years as potential emissions (i.e. about 99% of metals) contrib-
uting to a “stored toxicity” impact category which, however, should
not be compared directly with the other impact categories covering
the more “current” impacts (Hauschild et al., 2008). In this study,
emissions after the 100 years time horizon were excluded; however,
as this decision equally affected all scenarios the importance for the
overall conclusions is considered insignificant for the ranking of
scenarios. Nevertheless, long-term leaching should always be
addressed in a risk assessment perspective when evaluating specific
installations.
5. Conclusions
No management alternative appeared significantly better than the
others in all LCA impact categories; however, the thermal treatment
processes appeared to have significantly larger environmental
impacts in non-toxicity categories than the remaining treatment
options. This was primarily due to the energy consumption in these
processes. A sensitivity analysis using natural gas instead of coal as
fuel for electricity production did not change this conclusion.
In toxicity related categories (primarily related to leaching and air
emissions), all alternatives performed significantly better than the
baseline case with landfilling of untreated residues; however, given
the uncertainties no individual management alternative could be
singled out as significantly better than the others. Again thermal
processes showed significant impacts from air emissions.
Transportation of residues to treatment and/or their final
destination contributed to increased impacts both in non-toxicity an
toxicity related categories; however, this did not alter the overall
balance between management alternatives.
Although considerable efforts were done in this study to obtain
and verify process data for the individual management alternatives,
the available documentation for these waste treatment techniques
was generally rather poor. Consequently, very detailed conclusions
regarding small differences between individual alternatives cannot be
justified. Overall, considering data uncertainties, thermal processes
came out worse due to energy consumptions and air emissions while
the remaining management alternatives (excluding direct landfilling)
came out better.
Acknowledgements
This study was based on several projects carried out at the
Technical University of Denmark throughout the last about 10 years.
4680 T. Fruergaard et al. / Science of the Total Environment 408 (2010) 4672–4680

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