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Journal of Cleaner Production 55 (2013) 72e83

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Journal of Cleaner Production


journal homepage: www.elsevier.com/locate/jclepro

Characterization of landfilled materials: screening of the enhanced


landfill mining potential
Mieke Quaghebeur a, *, Ben Laenen a, Daneel Geysen b, Peter Nielsen a,
Yiannis Pontikes b, Tom Van Gerven c, Jeroen Spooren a
a
Separation and Conversion Technology, VITO, Boeretang 200, 2400 Mol, Belgium
b
Department of Metallurgy and Materials Engineering, K.U. Leuven, Kasteelpark Arenberg 44, 3001 Heverlee, Belgium
c
Department of Chemical Engineering, K.U. Leuven, de Croylaan 46, 3001 Heverlee, Belgium

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

Article history: The main objective of “Enhanced landfill mining” is the valorization of the excavated waste materials that
Received 30 May 2011 have been stored in the landfill. Previous landfill mining projects have shown that each landfill site has
Received in revised form its own potential with regard to landfill mining. Factors such as the age of the landfill, type of landfill and
8 June 2012
the country or region where the landfill is located might have an impact on the type of materials stored
Accepted 19 June 2012
Available online 3 July 2012
in the landfill and their valorization potential. In the present article, the valorization options for the
materials stored at the REMO site in Houthalen (Belgium) are assessed based on excavation tests done at
locations containing either municipal solid waste (MSW) or industrial waste (IW). The results reveal
Keywords:
Enhanced landfill mining
differences in the composition and the characteristics of the waste materials with regard to type of waste
Resource recovery (MSW versus IW) and the period during which the waste was stored. Based on the characteristics of the
Recycling of mixed waste streams different fractions, an initial assessment was made with regard to their valorization potential. For the
plastics, paper/cardboard, wood and textile recovered in this study, waste-to-energy is the most suitable
valorization route since the level of contamination was too high to allow high quality material recycling.
For metals, glass/ceramics, stones and other inerts in the waste, material valorization might be possible
when the materials can adequately be separated. The amount of combustible in the excavated waste
varied between 23 and 50% (w/w) with a calorific value of around 18 MJ kg1 dw and confirm the large
potential of waste-to-energy for landfill mining. All waste samples recovered from the landfill contained
a large amount (40e60% (w/w)) of a fine grained (<10 mm) mainly mineral waste material. Especially for
industrial waste (mainly shredder from ELV), the fines contained high concentrations of heavy metals
(Cu, Cr, Ni and Zn) and offer opportunities for metal extraction and recovery. The development of
a treatment plant that enables maximum resource recovery remains however one of the technological
challenges for further development of enhanced landfill mining.
Ó 2012 Elsevier Ltd. All rights reserved.

1. Introduction high quality recycled aggregates and waste derived fuels. Both the
legislative framework and increasing market prices for the recycled
In the last decade new technologies and processes have materials create conditions that justify the development of new
emerged that enable more efficient recycling of materials from waste recycling and separation technologies (Archer et al., 2005;
often complex and heterogeneous waste streams (Simonds, 1999; Forton et al., 2006; Tachwali et al., 2007).
Archer et al., 2005; Cossu and Gadia, 2007). The principal drivers for Recently, the concept of Enhanced Landfill Mining (ELFM) has
these developments are the local and EU legislation on waste been proposed as an improved practice of landfill mining. Essen-
(Directive 2008/98/EC), as well as the growing demand for metals, tially, ELFM includes the combined and integrated valorization of
(historic and future) waste streams as both materials (Waste-to-
Material, WtM) and energy (Waste-to-Energy, WtE), while
* Corresponding author. Tel.: þ32 14335646; fax: þ32 14321186. respecting stringent ecological and social criteria (Jones et al.,
E-mail addresses: mieke.quaghebeur@vito.be (M. Quaghebeur), ben.laenen@
vito.be (B. Laenen), daneel.geysen@mtm.kuleuven.be (D. Geysen), peter.nielsen@
accepted for publication). One of the main drivers of “Enhanced
vito.be (P. Nielsen), yiannis.pontikes@mtm.kuleuven.be (Y. Pontikes), landfill mining” (ELFM) is the valorization of waste materials
tom.vangerven@cit.kuleuven.be (T. Van Gerven), jeroen.spooren@vito.be (J. Spooren). excavated from landfills. Due to the heterogeneous nature of the

0959-6526/$ e see front matter Ó 2012 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.jclepro.2012.06.012
M. Quaghebeur et al. / Journal of Cleaner Production 55 (2013) 72e83 73

waste streams in landfills, separation and treatment of the different records provide no detailed information with regard to the physico-
waste streams are required to enable the generation of valuable chemical properties of the waste necessary to assess the valoriza-
(recycled) materials. Specific treatment and separation schemes are tion potential, an exploratory field test was carried out at the REMO
available for the treatment of various specific (often) heterogeneous site. The objectives of the field test were to:
waste streams such as shredder residue, bottom ash, C&D waste and
contaminated soil. Most of these schemes make use of a combina-  Evaluate differences in composition of the waste with regard to
tion of dry and/or wet mechanical separation techniques including the type of waste stored (household versus industrial waste);
crushing, milling, sieving, magnetic and eddy current separation of  Assess the variation in composition for each specific waste
ferrous and non-ferrous metals, density separation based on air type;
flow, water based density separation techniques, jigging, etc. In  Investigate the impact of storage time on the composition and
case of ELFM, the treatment plant should be able to recover high characteristics of the waste;
quality waste fuel and materials (e.g., ferro and non-ferro metals)  Compare the composition of the waste with data available in
from a mixture of heterogeneous waste streams of which the the records and in literature;
composition and hence the physical and chemical properties are  Make an assessment of the valorization potential of the
influenced by the age of the waste and the degradation of the waste materials stored in the landfill.
over time. Part of the waste streams are even residues from mixtures
of the residual waste originating from elaborated treatment 2. Materials and methods
schemes that were designed in the past to recover and recycle
materials from specific waste streams. The development of a sepa- 2.1. Site description
ration plant that enables maximum resource recovery is one of the
technological challenges of enhanced landfill mining. The REMO landfill has been in operation since the start of the
Previous pilot and pre-feasibility studies around the world as 1970s and is located in Houthalen-Helchteren in the province of
well as completed landfill mining projects have shown that Limburg in Belgium. The total area of the landfill containing non-
different landfill sites have different potential with regard to hazardous waste that is considered for enhanced landfill mining
landfill mining. Factors such as the age of the landfill, type of is about 1.286.200 m2. The landfill has been divided into sections
landfill, meteorological, hydrological conditions and the country or based on the type of waste stored, the period during which the
region where the landfill is located might have an impact on the section was in operation and the location in the landfill. For each
type of materials stored in the landfill and their valorization section information is available with regard to the type and amount
potential. To determine the recycling potential for a specific landfill, of waste stored. Roughly half of the 16.5 million tons that have been
quantitative and qualitative analysis of the waste streams stored landfilled at REMO is household waste. The other half comprises
are essential (Prechthai et al., 2008). industrial waste such as shredder material from the ELV recycling,
The Closing the Circle project (CtC) in Houthalen-Helchteren metallurgical slags, pyrite containing slags, dried sludge, etc.
(Belgium) is the first ELFM case study. The feasibility of the CtC/ Leachate collection and treatment, soil protection measurements
ELFM was investigated through several studies and analysis. The and methane recovery are in place and comply with the Flemish
impact on biodiversity and recovery of natural land is described by and European legislation (VLAREM, landfill Directive/1999/31/EC).
De Vocht and Descamps (2011). The economic feasibility of ELFM
was explored and special attention was given to the environmental 2.2. Excavation and sampling procedure
impact through the calculation of the carbon footprint (Van Passel
et al., accepted for publication). Although it is clear that all these An important aspect of the field test was the design of the
aspects are important, the feasibility of ELFM will also be deter- sampling procedure. Several sampling methods were considered,
mined by the quality of the materials retained in the landfill and the however, due to the high costs related to the excavation and analysis
WtM and WtE technologies available for valorization. Therefore, of the samples a more practical approach was followed taking into
this paper focuses on the characteristics and the valorization account the information available with regard to the different
potential of the waste streams stored at the REMO site in sections in the landfill. It was therefore decided to test 6 different
Houthalen-Helchteren (Belgium) obtained during an exploratory locations in detail during the field test. An overview of the type of
field test (EFRO-project 475, 2010e2011). At the REMO site around waste and the time of disposal at a specific location is given in Table 1.
15 million tons of waste have been landfilled since the beginning of The selection of the test locations was based on the type of waste and
the 1970s. Both household and industrial wastes have been land- the period during which the waste was stored. For municipal solid
filled. Records are available specifying the amount, the type and the waste (MSW), the aim was to select 4 locations that varied with
location of the different waste streams within the landfill. Since the regard to the period during which the waste was generated. The

Table 1
Description of the waste samples taken at the selected sampling locationsof the field test.

Number Year of storage Type of waste Top liner Bottom liner Description of waste Depth of landfill (m)
1 1980e1985 MSW 1 m clay þ 1 m soil Clay Municipal solid waste originating from both 11
households, businesses and industrial companies
2 1985e1990 MSW 1 m clay þ 1 m soil Clay þ 2 mm foil Municipal solid waste originating from 13
businesses and industrial companies
3 1990e1995 MSW 1 m clay þ 1 m soil Clay þ 2.5 mm foil Municipal solid waste originating from 11
businesses and industrial companies
4 1995e2000 IW 1 m clay þ 1 m soil Clay þ 2.5 mm foil Industrial waste rich in shredder and fine 9
residues such as sludge
5 1985e1990 IW 1 m clay þ 1 m soil Clay þ 2 mm foil Industrial waste 8
6 1995e2000 MSW 1 m clay þ 1 m soil Clay þ 2.5 mm foil Municipal solid waste originating from 13
businesses and industrial companies
74 M. Quaghebeur et al. / Journal of Cleaner Production 55 (2013) 72e83

maximum storage time of the MSW varied between 14 and 29 years composition (e.g., volatilization of organic compounds or melting of
and the locations were chosen to collect data that are representative plastics retained in the waste). Initial tests, however, showed that
for the majority of the municipal solid wastes stored at the REMO a drying temperature of 40  C resulted in very long drying periods
site. For industrial waste only 2 locations were investigated of which (7e10 days) for the large samples (20e30 L) of excavated waste.
the maximum storage time of the waste varied between 14 and 24 Since the temperature inside a landfill is known to increase up
years. Since a variety of industrial waste materials have been stored 90  C (Klein et al., 2001) it was decided to determine the moisture
at the REMO site, it was decided to focus on the locations rich in old content of the waste samples by drying the samples in a ventilated
and more recent shredder-like waste. Locations rich in metallurgical oven at 70  C for 48 h. Each of the dried samples was then screened
slag, pyrite containing slag, MSWI-bottom ash, sludge, etc.were with a sieve mesh of 10 mm. Subsequently, the composition of the
therefore not investigated in this study. It is clear that for IW the oversized fraction was determined by manual sorting into 8 sub-
exploratory field test was carried out to get a first impression of the fractions (plastics, textile, wood, paper/cardboard, metal, glass/
variability of the landfill but that more research is needed to ensure ceramics, stone and an undefined fraction). The weight of the
a complete characterization of the landfill. different sub-fractions was determined and the physical and
A cactus grab crane was used to collect the waste samples up to chemical composition of a number of representative samples were
the maximum depth of the landfill (Fig. 1). A shaft of about 1  1 m analyzed after size reduction. An overview of the sample treatment
and up to 15 m deep was excavated at each location where waste scheme is presented in Fig. 2. In addition to the analysis of the
samples were collected at each depth interval (0e1 m, 1e2 m,.) in individual separated fractions, the chemical and physical properties
the bucket of a wheel loader. This sample was subsequently loaded of some of the non-sorted waste samples were also determined. For
into a container in which the sample was mixed and spread out in waste-to-energy applications characteristics such as moisture
a thin layer at the bottom of the container. Oversized (>200 mm) content, ash content, calorific value and amount of organic carbon,
objects such as boulders, metal bars and very large sheets of plastic total carbon (C), hydrogen (H) and nitrogen (N) are needed to assess
were separated from the bulk sample and their volume/mass the efficiency. In addition the amount of sulfur (S), chlorine (Cl),
percentage was estimated and recorded. To collect a representative fluorine (F) and bromine (Br) of the waste is needed to control the
sample from each container, a grid was placed on top of the waste amount of emission levels during thermal conversion. The inor-
layer. The composition of the waste samples from two grid cells (see ganic composition of certain fractions was analyzed to evaluate the
Fig. 1) was described by visual inspection without detailed sorting. waste-to-material valorization options.
The waste samples were then stored in closed plastic buckets (30 L). The dry weight of the samples was analyzed according to CEN/
During the field excavation tests around 130 samples were collected TS 15414:2006. The ash content was determined at 550  C and
of which 38 samples were investigated in detail. 815  C according to CEN/TS 15403: 2006. The gross and net caloric
values were analyzed at constant pressure according to CEN/TS
2.3. Composition and characterization of the waste 15400:2006. Carbon (C), hydrogen (H) and nitrogen (N) were
determined using CEN/TS 15407:2006 while sulfur (S), chlorine
For most environmental analysis, soil and waste samples need (Cl), fluorine (F) and bromine (Br) were analyzed using CEN/TS
to be dried at low temperature (<40  C) to avoid changes in 15408:2006. TOC was determined with the Ströhlein TOC-analyzer

Fig. 1. Overview of sampling method used at the REMO closed landfill site. A cactus grab crane was used to collect the waste samples up to the maximum depth of the landfill (A). A
shaft of about 1  1 m and up to 15 m deep was excavated at each location during which waste samples were collected at each depth interval (0e1 m, 1e2 m,.) in the bucket of
a wheel loader (B). This sample was subsequently loaded into a container (C) in which the sample was mixed and spread out in a thin layer at the bottom of the container (D).
M. Quaghebeur et al. / Journal of Cleaner Production 55 (2013) 72e83 75

Fig. 2. Schematic representation of the sample pretreatment procedure to determine the composition and physical and chemical characteristics of the excavated samples.

C-mat 5500 according to EN13137: 2001.EOX was determined composition of the initially landfilled waste resulting from differ-
according to the local CMA procedure CMA/3/N (based on NEN ences in waste management procedures, legislation or changes in
5735), while the inorganic composition of the samples (Al, Ca, P, Fe, the type of goods produced and consumed during a specific period.
Mg, Mn, Na, Si, Ti, As, Cd, Cr, Ni, Cu, Hg, Pb, Zn, Te, Sn, Ba, Mn, Mo, Due to the large standard deviation, confirmation of the trend is
Se, Sr and V) was analyzed using microwave assisted digestion needed by comparison with independent data. In the Flemish region
with acid (HF/HNO3/HCl) with subsequent analysis by ICP-AES or of Belgium data on the composition of fresh municipal solid waste
ICP-OES (EN13656: 2002). have been gathered since 1993 (OVAM, 2003). In the OVAM study,
the average composition of municipal solid waste collected was
3. Results and discussion typically based on the analyses of up to 2000 samples (total weight
equals to 13 ton) collected all across the Flemish region (Table 2). At
3.1. Composition of the waste material the REMO site, the amount of plastic increased from 10 to 25% (w/w)
for MSW initially landfilled between 1980 and 2000. This increase
3.1.1. Influence between type of waste material and composition probably reflects an increase in production and consumption of
In Fig. 3 an overview is given of the composition of the waste plastic during this period. Analysis of the composition of fresh
excavated at each location. Since no trend could be observed in the household waste sampled between 1993 and 2000 also showed an
composition of the waste with increasing depth of the landfill (data increase in the amount of plastic (from 17 to 24% (w/w)) (OVAM,
not shown), average values and standard deviations are presented in 2003) (Table 2). The decrease in metal content (4.3e2.2% (w/w))
Fig. 3. Significant differences in composition could be observed and the content of glass/ceramic (1.7e0.5% (w/w)) over time in
between the MSW and the IW. Although the main fraction in both MSW is most likely also caused by changes in the composition of
the MSW and the IW was a fine soil type waste fraction, the amount the fresh waste as confirmed by the Flemish records (OVAM,
present in the IW (64  16% (w/w)) was significantly higher than that 2003). For the paper/cardboard content, the difference from 4 to
in the MSW (44  12% (w/w)) based on dry sieving with a mesh of 14% (w/w) between waste landfilled in 1980 and 2000 can most
10 mm. The composition of the fine fraction could not be described in likely be attributed to degradation of the material in the landfill over
detail without further analysis. It is however clear that for the MSW, time. Especially since based on the Flemish records, the content of
part of the fine fraction is composed of degraded garden and food paper/cardboard in fresh household waste seems to decrease
materials. The amount of plastic, paper/cardboard and textile was slightly in more recent years (Table 2). Since only two locations were
higher in the MSW compared to the IW. It is clear that the compo- investigated for IW, no detailed analysis could be carried out with
sition of MSW is significantly different compared to the shredder- regard to changes in the composition of IW over time.
like IW examined in this study. During the manual separation test Few studies exist in which the influence of storage time on the
both MSW and IW contained respectively 4  4% (w/w) and 8  6% composition of excavated waste is examined. The results in this
(w/w) of an unknown fraction of which the origin could not be study show that for most fractions (metals, plastics, glass/ceramics,
determined by visual inspection. Chemical analysis revealed that the stones and textile) the amount found in excavated waste is
unknown fraction was most likely a mixture of degraded organic comparable to the amount originally present in the waste when it
materials and sand (further results not included in this study). No was initially landfilled (Table 2). For MSW, records with regard to
unexpected hazardous materials were excavated in this study. the composition of fresh waste over time are therefore a good
source of information to estimate the composition of landfilled
3.1.2. Influence of storage time in the landfill and composition of the waste. The organic waste (food, vegetables, garden waste,.)
waste cannot be distinguished after 15 years of landfilling. The material
For MSW, information on the composition of waste samples degrades and is transformed into a fine soil like fraction. Also
stored during a period of 14, 19, 24, 29 year is available. Although the paper/cardboard seems to degrade over time. The exploratory field
standard deviation of the average content of the individual fractions test in the REMO site also revealed that the composition of exca-
is large, trends can be observed for some fractions with regard to vated MSW changed with regard to the period (1980e2000) during
changes over time. These changes can be attributed to degradation/ which the waste was landfilled. Especially the changes in amount of
decomposition of the waste over time or due to differences in the plastics and metals over time (and to a lesser degree also changes in
76 M. Quaghebeur et al. / Journal of Cleaner Production 55 (2013) 72e83

Fig. 3. Average composition and moisture content of municipal solid waste and industrial waste that had been stored in the REMO landfill for between 9 and 29 years. For each
weight percentage a standard deviation is indicated by an error bar.

organic waste, paper/cardboard and textile) might have an impact recycling practices, cultural and consumer habits, standard of
on the materials and amount of energy that can be recovered from living, etc. (Thitame et al., 2010; Abu-Qudais and Abu-Qdais,
excavated MSW. 2000). Few studies have however investigated the composition of
excavated MSW after landfilling (Hogland et al., 2004; Kurian et al.,
3.1.3. Influence of geographic origin on composition of the waste 2004; Prechthai et al., 2008). Variations in the composition of
It is known that the composition of MSW will change according excavated waste can be observed between waste excavated from
to the geographic region where the waste is generated (UNEP, a landfill in Sweden, Thailand and Belgium (Table 3). The amount of
2004). This has been explained by differences in waste legislation, combustibles (plastics, textile, wood and paper) varied between 21
M. Quaghebeur et al. / Journal of Cleaner Production 55 (2013) 72e83 77

Table 2
Average composition of fresh MSW sampled in the Flemish region of Belgium in the period 1993e2001 (OVAM, 2003). The composition at each period is based on manual
separation of up to 2000 fresh MSW samples collected in the Flemish region. The average composition of fresh MSW in the period 1994e2001 was compared with the average
composition of excavated MSW at location 6 of the REMO landfill as analyzed in this study. For the fresh waste the composition is based on the analysis of 6 samples. The
standard deviation is given between parentheses.

Fresh MSW (OVAM, 2003) Excavated MSW (location 6, REMO)

2000e2001 1995e1996 1994e1995 1993e1994 1994e2001 1995e2000


Organic waste 43 48 48 49 47 (3) e
Soil e e e e e 45 (18)
Wood e e e e e 4.1 (4)
Paper/cardboard 14 18 18 16 17 (2) 14 (8)
Glass 2.4 3.2 4.1 3.8 3 (0.8) 0.5 ()
Metals 3.2 3.9 4.1 3.7 4 (0.4) 2.2 (2)
Plastics 24 17 17.0 17 16 (7) 25 (13)
Textile 2.9 2.2 2.4 3.0 3 (0.4) 3.1 (5)
Hazardeous waste 0.68 0.87 0.55 0.55 1 (0.2) e
Inert fraction 3.3 3.6 2.2 4.4 3 (0.9) 2.0 (6)
Rest 5.9 3.6 2.8 2.0 4 (2) 4.1 (4)

and 50% (w/w). The content of inerts (glass/ceramics and stones) 18.8 MJ kg1 dw (UNEP, 2009)). For glass/ceramic, metal and stone
varied between 10 and 17% (w/w) while the amount of soil type the calorific value and the TOC content were neglected.
material ranged between 34 and 60% (w/w). For metals the content As illustrated in Fig. 4, the calorific value and the TOC concen-
varied between 3 and 6% (w/w). trations in MSW decreased respectively from 11.8 to 6.7 MJ kg1 dw
The average moisture content of the waste samples excavated at and 28 to 19% (w/w) with increasing storage time in the landfill.
one location at the REMO landfill varied between 48 and 66% (w/w) This decrease is most likely the result of decomposition of C-rich
and is comparable to previous reported values (Hogland et al., material into landfill gas over time. Landfill gas is the mixture of
2004; Prechthai et al., 2008). During the excavation test it was carbon dioxide and methane, and other trace components, gener-
observed that the moisture content in the landfill varied signifi- ated by biological decomposition of organic waste. At the REMO
cantly due to the presence of poor-draining or impervious layers in landfill, methane gas is collected in the landfill and converted to
the landfill. Some layers were saturated with water, while other electrical energy. The most important factors that affect methane
regions in the near vicinity were dry. For each location large generation include waste composition, moisture content, temper-
difference in moisture content were indeed observed with regard ature, waste nutrient level, and the presence or absence of buffering
to the depth of the landfill (standard deviation between 10 and agents (which may be provided from sources such as cover soils). It
48%). The water balance of the landfill and hence the moisture is therefore clear that the degradation varies significantly between
content of the excavated waste can vary significantly and need to be different landfills as well as inside each landfill. In this study, the
taken into consideration when evaluating the valorization and average degradation could be described reasonably well with a first
treatment options for enhanced landfill mining. order decay curve [C(t) ¼ C0 ekt; R2 ¼ 0.98, C0 ¼ 42%;
k ¼ 0.0269 year1] (Fig. 3). The factor ‘k’ is the first order rate
3.2. Degradation of the waste material: changes in calorific value constant and reflects the rate at which the degradation of carbon-
and total amount of waste rich material occurs. The estimated value can be compared to the
first order rate constant often used in models to predict methane
For MSW the average calorific value and the average TOC content recovery from landfills. Although various types of models are
of the waste excavated at the 4 locations were calculated using the available (Vogt and Augenstein, 1997), simple first order models
individual material fractions (<10 mm, plastic, paper/cardboard, have been used successfully to describe and predict landfill gas
wood, textile, glass/ceramic, metal and stone) at each location generation (Vroonhof and Croezen, 2006) with k-values ranging
(Fig. 3) and the calorific value and the TOC content of the individual between 0.02 year1 en 0.10 year1. The factor ‘C0’ represents the
material fractions. For plastic, paper/cardboard, wood fractions and concentration of TOC in the MSW at the time of burial. Despite the
the fines (<10 mm), measured TOC and calorific values were used heterogeneity of the organic matter content of fresh organic MSW,
(see paragraph 3.4). For textile values from literature were used several studies have shown that in Europe the average TOC is
(TOC-content 55% (w/w) (UNEP, 2009), calorific value constant around 43e44% (w/w) (Baky and Eriksson, 2003; Jiménez

Table 3
Comparison of the average composition of excavated MSW from this field test with that of other landfill mining studies. For Sweden the average composition of the waste from
the Masalycke and Gladsax landfill were used as reported by Hogland et al. (2004). For Thailand the average composition of excavated waste from the Nonthaburi dump was
used as reported by Prechthai et al. (2008). The standard deviation is given between parentheses. The number of samples (N) analyzed during each study is indicated.

Country (age) Reference Thailand (3e5 years old) Sweden (17e25 year old) Belgium (14e29 years old)
Number of samples (N) Prechthai et al. (2008) Hogland et al. (2004) This study

12 6 23
Glass 6.5 0.5 (1) 1.3 (0.8)
Inert fraction (stone) 3.3 16 (9) 10 (6)
Metal 6.4 1.6 (0.4) 2.8 (1)
Textile 7.6 1.8 (2) 6.8 (6)
Wood 8 7.2 (5) 6.7 (5)
Paper/cardboard 3.3 7.2 (7) 7.5 (6)
Plastic/rubber/foam 31 4.4 (3) 17 (10)
Soil 34 60 (13) 44 (12)
78 M. Quaghebeur et al. / Journal of Cleaner Production 55 (2013) 72e83

fine fraction separated from waste by Hogland et al. (2004). The


calorific value and the TOC concentration for the soil like MSW
seem higher than those for the fine fraction IW. In addition, the
calorific value (2.2e4.8 MJ kg1 dw) and the TOC concentration
(7.6e12% (w/w)) decreased with increasing storage time of the
MSW. A large portion of the organic carbon in the soil like fraction
has been converted and recovered as landfill gas during storage in
the REMO landfill. Further stabilization of the organic matter by
composting the soil type fraction after excavation was therefore
not considered in this study. In Sweden lower calorific values
(0.4e0.9 MJ kg1) were reported for fines screened from waste that
had been landfilled for a period of 14 years (Hogland et al., 2004).
The concentrations of major and minor elements determined in
the fine, soil type fraction are presented in Table 5. The average
chemical composition of the fine fraction separated from IW clearly
contains more Ca, Fe and metals such as Cr, Cu, Ni, Pb and Zn
compared to the soil type fraction originating from MSW. For MSW,
Fig. 4. Relation between average TOC concentration and maximum storage time of the a decrease in the concentration of As, Cd, Cr, Cu, Hg, Ni, Pb and Zn
“soil type” waste fraction separated from MSW at the REMO landfill (left axis). with decreasing storage time could be observed and can most likely
Correlation between the calorific value (right axis) and the average TOC concentration
be attributed to an improved initial quality of the fresh MSW that
for the “soil type” waste fractions separated from excavated MSW and IW landfilled
between 1980 and 2000 at the REMO site. has been landfilled over time. The concentrations of heavy metals
in the fine fraction of MSW investigated in this study are generally
higher compared to the values reported for a landfill mining study
and Garcia (1992)). The fact that the value for C0 obtained in this in Sweden (Hogland et al., 1995) but are in agreement with values
study (42% (w/w)) is similar to the reported values in literature reported for a landfill site in Thailand (Prechthai et al., 2008). A
suggests that the methodology and the sampling procedures used magnet was subsequently used to determine the amount of ferrous
for MSW in this exploratory field test were adequate and metals in the soil type fraction. The magnetic fraction in the fine
representative. fraction from IW was significantly higher (25e29% (w/w)) than the
The decay curve was subsequently used to calculate the amount magnetic fraction from MSW (0.5e5.3% (w/w)).
of MSW waste that was lost during degradation. Data available with For MSW, an increase in the amount of magnetic material was
regard to type, amount and period during which the waste was observed with increasing age of the waste. Since the magnetic
landfilled at a specific location in the REMO landfill was used as fraction separated from the soil type fraction was still a mixture of
input. Calculations predict that from the 7.5 million ton dry MSW metals, oxides and other minerals, XRF analysis after ignition
(10.2 million ton wet) initially landfilled, approximately 1.5 million combined with microscopic analyses was used to determine the
ton dry organic matter (or 20% (w/w)) was lost during landfilling. amount and speciation of the metals present in the magnetic frac-
tion (data not presented). The amount of metallic iron in the
3.3. Characterization of fraction <10 mm magnetic fraction was estimated to be between 8 and 9% (w/w) with
the metallic iron often embedded in an oxide-rich matrix (Fig. 5).
The fraction <10 mm is the major fraction in both MSW and IW
and is composed of all the waste materials that pass through a sieve
with a mesh size of 10 mm. Due to the unknown and heterogeneous 3.4. Characteristics of plastics
nature of the material, this fine, soil type fraction was analyzed in
detail. The results of the properties relevant for energy recovery The plastic fraction is characterized by an elevated ash content
and material valorization are presented in Tables 4 and 5. (20e35% (w/w)) and a lower calorific value (19e28 MJ kg1)
The ash content for MSW seems generally lower than the ash compared to the ash content and calorific value of mixed plastic
content for IW and is comparable to the ash content reported for the streams reported in literature (Phyllis database) (ash content: 1%;

Table 4
Average characteristics of the soil type waste fraction (<10 mm) separated from waste samples excavated at the REMO site during the field test. The standard deviation is given
between parentheses. The number of samples (N) on which each result is based is indicated.

Location 1 2 3 6 5 4

Type MSW MSW MSW MSW IW IW

Age 1980e1985 1985e1990 1990e1995 1995e2000 1985e1990 1995e2000

Number of samples (N) 2 2 1 2 1 2


Ashcontent (815  C) 85 (7) 77 (2) 64.4 80.9 (5) 87.50 85.2 (2)
Total carbon (%) 7.8 (5) 11 (0.8) 14.7 11.3 (5) 5.93 7.1 (5)
TOC (%) 7.6 (3) 9.5 (0.4) 12 12.4 (5) 4.60 5.4 (3)
Hydrogen (H) (%) 0.88 (0) 1.2 (0.1) 1.7 1.1 (0.1) 0.81 1.2 (0.2)
Nitrogen (N) (%) 0.39 (0.2) 0.53 (0.0) 0.66 0.39 (0.1) 0.30 0.28 (0.1)
Net calorific value (MJ kg1 dw) 2.2 (0.7) 3.2 (0.5) 4.7 4.8 (2) 1.30 2.0 (2)
Bruto calorific value (MJ kg1 dw) 2.4 (0.8) 3.4 (0.6) 5.7 5.0 (2) 2.30 2.1 (2)
Bromide (%) 0.03 (0) 0.03 (0.0) 0.03 0.03 (0.0) 0.03 0.03 (0)
Chloride (%) 0.15 (0.02) 0.41 (0.2) 0.26 0.26 (0.2) 0.17 0.36 (0.09)
Fluoride (%) 0.009 (0.005) 0.01 (0.0) 0.01 0.02 (0.0) 0.30 0.38 (0.5)
Sulfur (%) 0.19 (0.1) 0.26 (0.1) 0.23 0.22 (0.1) 0.31 1.5 (2)
M. Quaghebeur et al. / Journal of Cleaner Production 55 (2013) 72e83 79

Table 5
Average concentrations of major and minor elements of the soil type waste fraction (<10 mm) separated from MSW and IW waste samples excavated at the REMO site during
the field test. In the bottom rows the limit values of the Flemish regulations VLAREA and VLAREBO for the heavy metals are given for comparison. The standard deviation is
given between parentheses. The number of samples (N) on which each result is based is indicated.

Nr Type Year N Si g/kg Ca g/kg Fe g/kg EOX als As mg/kg Cd mg/kg Cr mg/kg Cu mg/kg Hg mg/kg Ni mg/kg Pb mg/kg Zn mg/kg
Cl mg/kg
1 MSW 1980e1985 2 260 (57) 31 (17) 34 (23) 715 (686) 61 (30) 8.5 (8) 770 (325) 285 (78) 2.0 (2) 335 (134) 500 (396) 670 (297)
2 MSW 1985e1990 2 235 (35) 35 (1) 39 (4) 960 (481) 31 (28) 8.4 (5) 380 (141) 205 (106) 0.50 (0.1) 164 (107) 310 (184) 735 (219)
3 MSW 1990e1995 1 220 () 33 () 18 () 670 () 7.2 () 3.3 () 720 () 760 () 0.27 () 160 () 180 () 800 ()
6 MSW 1995e2000 2 243 (6) 14 (7) 17 (3) 1787 (2872) 9.1 (2) 3.3 (2) 113 (6) 107 (37) 0.19 (0.1) 46 (2) 172 (89) 463 (329)
5 IW 1985e1990 1 230 () 73 () 53 () 410 () 19 () 15 () 3800 () 1200 () 2.4 () 2200 () 1100 () 2600 ()
4 IW 1995e2000 2 181 (126) 78 (88) 54 (8) 284 (334) 22 (6) 19 (1) 5730 (7453) 5750 (6010) 0.99 (1) 4640 (6166) 2640 (2489) 5600 (849)

VLAREBO limit values unrestricted use of soil (mg/kg)a 19 2.6 91 135 1.7 56 120 529
VLAREBO limit values for contaminated soil (type III) (mg/kg)a 103 6 240 396 4.8 95 560 881
VLAREBO limit values for use of soil in or as 250 10 880 375 5 250 1250 1250
construction material (mg/kg)
VLAREA limit values for use of waste as soil 150 6 250 375 5 50 300 900
fertilizer and compost (mg/kg)
VLAREA guidance value for use of waste in or 250 10 1250 375 5 250 1250 1250
as construction materials (mg/kg)
a
Calculated with 2% clay, 10% OM and pH 7.

calorific value: 35 MJ kg1 (Table 6). Since the plastics were sepa- (Table 8). The TOC concentration varies between 25 and 34% (w/w)
rated from the waste by handpicking without further washing or and is comparable to the TOC concentration reported for paper in
treatment it is likely that some dust or sand particles sticking to the MSW (27% (w/w)) (Agentschap NL, 2010). The net calorific value
plastics influenced the measurements. The chloride concentration varied between 6,7 and 12 MJ kg1 dw and is slightly lower than the
varied between 0.5 and 7.3% (w/w). caloric value reported for mixed paper streams (15 MJ kg1 dw).
In this study, no differences could be observed in TOC concen- The metal concentration is generally lower than the concentration
tration and calorific value between the plastic fraction separated reported for the plastic fraction (Table 9).
from IW versus MSW. The amount of TOC compares well with the
values reported for plastics in MSW in the Netherlands (59% (w/w)) 3.6. Valorization options
(Agentschap NL, 2010). The plastic fraction separated from IW,
seems to contain higher concentrations of metals such as Ba, Cd, Cr, Based on the characteristics of the individual fractions separated
Cu, Pb and Zn compared to the plastic fraction from MSW (Table 7). from the waste, the valorization options were assessed. It should
The concentrations of heavy metals in the plastics recovered from however be taken into account that handpicking was used in this
MSW in this study were up to factor 10 high compared to the values study to separate individual fractions from the original waste
reported in other studies (Prechthai et al., 2008; He et al., 2006; samples. During full scale excavation of the landfill, a specific
Riber et al., 2005). No indication was found that the calorific value treatment plant will be designed to treat and separate the waste
of the plastic waste is influenced by degradation of the plastic which could result in different characteristics (ash content, chem-
during storage since no change in calorific value with increasing ical composition,.) or level of contamination compared to the
storage time of the plastic waste could be observed. It is known that fractions obtained during this study by handpicking. Although
plastics are very durable and degrade little during landfilling (Shah a variety of industrial waste materials have been stored at the
et al., 2008). REMO site, only locations rich in shredder type waste were inves-
tigated in the field test. For IW only the valorization options for
3.5. Characterization of paper/cardboard shredder type waste material will therefore be evaluated.

Only the paper/cardboard fractions separated from MSW were 3.6.1. Fine soil type fraction
analyzed in this study. The paper/cardboard fraction was charac- For both IW and MSW more than 40% (w/w) of the waste
terized by a high and variable ash content (25e61% (w/w)) material was classified as a “fine soil type fraction”. Since this

Fig. 5. Photomicrographs of thin-sections from the magnetic fraction of the soil type waste fractions showing details of a metallic Fe particle embedded by iron-oxide from IW
landfilled in 1995e2000 (left) and IW landfilled in 1985e1990 (right).
80 M. Quaghebeur et al. / Journal of Cleaner Production 55 (2013) 72e83

Table 6
Average characteristics with standard deviation (between parentheses) of the plastics separated from waste samples excavated at the REMO site during the field test. The
number of samples (N) on which each result is based is indicated.

Location 1 2 3 6 5 4

Type MSW MSW MSW MSW IW IW

Age 1980e1985 1985e1990 1990e1995 1995e2000 1985e1990 1995e2000

Number of samples (N) 3 1 1 2 1 1


Ashcontent (815  C) 25 (2) 32 38 20 23 35 (2)
Total carbon (%) 50 (2) 44 41 59 57 39 (7)
TOC (%) 57 (4) 51 53 67 58 37 (16)
Hydrogen (H) (%) 6.7 (1) 7 6.0 8.1 6.9 5.4 (0.2)
Nitrogen (N) (%) 0.7 (0) 1 0.59 0.2 0.7 0.75 (0.5)
Net calorific value (MJ kg1 dw) 24 (3) 21 18 27 26 21 (4)
Bruto calorific value (MJ kg1 dw) 25 (3) 23 19 28 28 22.1 (4)
Bromide (%) <0.025 () <0.025 <0.025 <0.025 <0.025 <0.025 ()
Chloride (%) 7.3 (3) 0 1.8 5.5 3.9 1.6 (1)
Fluoride (%) 0.01 (0) 0 0.006 0.0 0.056 0.061 (0.03)
Sulfur (%) 0.2 (0) 0 0.27 0.2 0.47 0.42 (0.01)

fraction is a combination of all the materials that pass through 3.6.2. Metals, glass/ceramic and stone
a 10 mm sieve further treatment and fractionation will be Although the characteristics of these fractions have not been
required to optimize the valorization of the materials contained presented in this paper, large part of these materials might be
in this fraction. Three valorization options can be considered: i.e. suitable for material valorization. Further research including
Waste-to-Energy, reuse as soil or construction material and metal leaching tests and determination of organic contaminants will be
recovery. Waste-to-Energy is based on the large amount of required to further assess and confirm the valorization routes. For
organic material (>10% for MSW; >8% for IW) present in this MSW, the metal fraction consists mainly of ferrous metals (75e84%
fraction. When the organic material is removed, the remaining (w/w)) while the remaining non-ferrous is mainly aluminum (>90%
material might be recycled as filler or construction material. It is, (w/w)) (OVAM, 2003). For IW, more variation can be expected.
however, clear that the quality of the fine fraction may not always
be suitable for material recovery because of elevated metal 3.6.3. Paper/cardboard, textile, wood and plastic
concentrations (Cd, Cr, Cu, Ni, Pb and Zn), especially in the fine For the plastic, textile, paper/cardboard and wood excavated
fraction from IW. One of the options is to reduce the concentra- from the landfill “Waste-to-Energy” with valorization of the resi-
tion (and later on recover) metals such as Cr, Cu, Ni, Zn, from the dues (e.g., slag, bottom ash) seems the most feasible valorization
fine fraction. Although only preliminary results are available, route. The quality and state of the textiles recovered from the
removal of the magnetic fraction could result in a reduction of the landfill, makes direct reuse as textile not an option. Also the paper/
concentration of metals by more than 50% (w/w). This can be cardboard, wood and plastic fractions are too heterogeneous or
explained by the high amount of metal-oxides associated with contaminated to make the fractions suitable for direct material
metallic iron (see Fig. 5). More research with regard to metal valorization. Technology to produce new paper/cardboard based on
recovery will be done in the future. For MSW, a decrease in the recycled paper is available and well established (Miranda and
concentration of As, Cd, Cr, Cu, Hg, Ni, Pb and Zn can be observed Blanco, 2010). Recycling of post-consumer paper is, however,
with decreasing storage time of the waste. For the most recent known to be problematic in paper pulping due to the high level of
landfilled MSW (1995e2000), the fine fraction might even be contamination (food, glass,.). In addition it is likely that the
valorized directly as soil fertilizer or compost without further degradation of the paper during storage in the landfill makes the
treatment. The metal concentrations in this fraction is below the paper unsuitable for production of new paper since the fiber length
Flemish limit values for use as soil fertilizer and compost is important in paper to paper recycling. Other material recycling
(VLAREA) and approach the Flemish limit values for unrestricted options include recycling as cellulosic insulation material (patent
reuse of excavated soil (VLAREBO, 2008) (Table 5). Further US7758719) or the use of paper pulp as pore forming agent in the
research including leaching tests and determination of the brick production (Huybrechts et al., 2008). The efficiency of the
concentrations of organic contaminants will be conducted on sub separation plant will determine to what extent material to material
fractions of the treated soil type fraction to further assess the routes might be feasible for paper/cardboard in the future.
valorization options. For the older MSW fines the concentrations With regard to material recycling of plastic, distinction can be
of Cd, Cr, Ni and Pb exceed the limit values for compost and hence made between primary, secondary and tertiary recycling (ASTM
further treatment is needed. D5033). Primary recycling is also called “closed-loop recycling” and

Table 7
Average concentrations of major and minor elements of the plastic fraction separated from MSW and IW waste samples excavated at the REMO site during the field test.

Nr Type Year Si g/kg Ca g/kg Fe g/kg EOX Cl As mg/kg Ba mg/kg Cd mg/kg Cr mg/kg Cu mg/kg Hg mg/kg Ni mg/kg Pb mg/kg Zn mg/kg
mg/kg
1 MSW 1980e1985 68 13 18 53,333 33 430 51 490 1767 0.6 327 550 1063
2 MSW 1985e1990 110 20 26 380 6.9 540 18 320 150 0.36 86 280 620
3 MSW 1990e1995 100 15 13 9600 6.2 600 19 280 690 0.46 73 230 1700
6 MSW 1995e2000 41 7.8 10 39,000 7.6 110 18 270 270 0.1 740 160 470
5 IW 1985e1990 72 26 23 3800 9.9 2300 47 780 10,000 2.0 640 1300 5500
4 IW 1995e2000 74 17.5 38 1860 12 3600 41 530 2405 1.1 275 1900 3800
M. Quaghebeur et al. / Journal of Cleaner Production 55 (2013) 72e83 81

Table 8 3.6.4. Resource mining: material and energy recuperation


Average characteristics of the paper/cardboard separated from waste samples It is well known that waste can be turned into valuable raw
excavated at the REMO site during the field test.
materials providing both environmental and economic benefits. In
Location 1 2 3 6 enhanced landfill mining the objective is to combine and integrate
Type MSW MSW MSW MSW the valorization of waste streams as both materials (Waste-to-
Material, WtM) and energy (Waste-to-Energy, WtE), while
Age 1980e1985 1985e1990 1990e1995 1995e2000
respecting stringent ecological and social criteria (Jones et al.,
Ashcontent (815  C) 43 61 25 35
Total carbon (%) 32 23 34 33
submitted for publication).
TOC (%) 34 25 33 31 Based on the characteristics of the individual fraction and
Hydrogen (H) (%) 3.9 2.6 4.0 3.7 the composition of the excavated MSW, the amount of combus-
Nitrogen (N) (%) 0.7 0.7 0.8 0.7 tibles (paper, textile, plastic and wood) varied between 34 and
Net calorific 11 6.7 12 12
50% (w/w) depending on the period during which the MSW was
value (MJ kg1 dw)
Bruto calorific 12 7.3 13 13 landfilled. The more recent the waste, the more combustible
value (MJ kg1 dw) materials it contained mainly due to the higher content of plastic
Bromide (%) <0.025 <0.025 <0.025 <0.025 in the fresh waste that was initially landfilled. The average
Chloride (%) 0.50 0.43 0.17 0.28
calorific value of the combustible fraction recovered from MSW
Fluoride (%) 0.01 0.01 0.01 0.01
Sulfur (%) 0.31 0.19 0.31 0.90
was 18.2  0.6 MJ kg1 dw and varied little between the locations
studied. The average ash content was 29  3% (w/w). It is
however possible that during full scale excavation of the landfill,
it can be described as mechanical recycling during which no a specific treatment plant will be used that is able to separate the
modifications occur in the chemical properties of the polymers. The combustibles more efficiently resulting in higher calorific values
plastic can therefore be used for the production of new products and lower ash contents. The other dominant fraction in excavated
without quality loss. Primary recycling is often limited to thermo- MSW is the soil like fraction which varied between 41 and 45%.
plastic polymers (PE, PP, PS,.) (melting and re-extrusion is often Although some further treatment might be required, this mate-
used) and post-industrial packaging waste. Post-consumer plastic rial might be reused as soil or construction material. In addition
is seldom recycled through re-extrusions because the level of the MSW contained an average content of 10  6% (w/w) stones,
contamination is mostly too high and the logistics involved in 1.3  0.8% (w/w) glass and 2.8  1% (w/w) metals that can be
collection/separation is challenging. Secondary recycling is also recycled as raw materials.
called “mechanical recycling with downgrading” and it involves Although a variety of industrial waste materials have been
a thorough washing, separation and mechanical treatment to be stored at the REMO site, only locations rich in shredder type
able to use the waste for the production of new plastic consumers waste were investigated in the field test. It is therefore only
goods such as piping, plastic bags, plastic chairs,.. Although possible to evaluate the valorization options for shredder type
secondary recycling might technically be feasible for some of the waste. The amount of combustibles in the shredder type waste
plastic recovered from the landfill it will be a challenge to make the (23  8% (w/w)) was rather low compared to that of MSW. The
process economically feasible taking into account the heteroge- calorific value of the combustibles was 18  2 MJ kg1 dw and the
neity and the quality of the plastic fraction recovered from the ash content was 35  5% (w/w). Most of the shredder type waste
landfill (Table 6). It should also be mentioned that a limit value of consisted of a soil like material (64  16% (w/w)) which contained
100 mg kg1 for heavy metals such as Pb, Cd, Hg and Cr(VI) is elevated concentrations of heavy metals like Cu, Cr, Ni and Zn.
stipulated in Europe for packaging material according to the Recovery of the metals combined with valorization of the mineral
Council Directive 94/62/EC with regard to packaging and packaging material as construction material will be investigated in the
waste. It is well known that elevated metal concentrations (e.g., Cd) future. In addition the shredder type waste contained an average
can be present in plastic recovered from landfill due to the type of content of 10  10% (w/w) stones, 0.05  0.04% (w/w) glass and
softeners, stabilizers and pigments used in plastic in the past 3.2  3% (w/w) metals that can be recycled as raw materials. It
(Prudent et al., 1996; Rotter et al., 2004). Taking into account the should however be mentioned that for the shredder type waste
elevated metal concentrations measured in the plastic recovered only 2 locations were investigated in detail so future research is
from the landfill (Table 7) it is unlikely that the excavated plastic recommended to confirm the data and obtain a more represen-
will be suitable for primary or secondary material recycling. tative assessment of the valorization potential of this waste
Tertiary or feedstock recycling of plastic uses depolymerization stream.
reactions to break up the polymers into smaller molecules, mostly Even though landfills are a potential for both energy and
gasses and liquids, that can be used as feedstock for the production material valorization, few landfills have been mined on commer-
of new plastics or petrochemical products (Al-Salem et al., 2009). cial basis so far. It is clear that both technological, economical and
Although, from a technical point of view, tertiary recycling might be legislative challenges exist in order to start full scale recovery of
a good option for plastic recovered from landfills, the number of resources from landfills (Van Passel et al., accepted for
industrial plants able to process plastic waste is still very limited in publication; Jones et al., accepted for publication; Krook et al.,
Europe. 2012).

Table 9
Average concentrations of major and minor elements of the paper/cardboard fraction separated from MSW waste samples excavated at the REMO site during the field test.

Nr Type Year Si g/kg Ca g/kg Fe g/kg EOX als Cl mg/kg As mg/kg Ba mg/kg Cd mg/kg Cr mg/kg Cu mg/kg Hg mg/kg Ni mg/kg Pb mg/kg Zn mg/kg
1 MSW 1980e1985 100 17 26 1300 39 240 1.4 310 150 0.45 120 440 900
2 MSW 1985e1990 130 32 29 640 9.7 480 16 200 210 0.27 56 330 560
3 MSW 1990e1995 88 27 6.5 270 4.9 180 <0.40 140 570 0.38 45 54 520
6 MSW 1995e2000 91 33 30 260 5.5 280 2.7 160 100 0.35 86 380 1900
82 M. Quaghebeur et al. / Journal of Cleaner Production 55 (2013) 72e83

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Mining (Extended Edition). Houthalen-Helchteren, pp. 275e290. 2010.
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characteristics of the waste materials stored at the REMO site based support from VEA).
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All waste samples recovered from the landfill contained a large Huishoudelijk afval sorteeranalyse-onderzoek 2000e2001, 2003. De Openbare
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Centre of the Netherlands.
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Acknowledgment production process. Waste Management 24, 1005e1021.
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for the funding of, respectively, the EFRO project proposal ‘Closing
lition Waste Management Practices, and Their Economic Impacts e Report by
the Circle, a demonstration of Enhanced Landfill Mining (ELFM)’ Symonds, in Association with ARGUS. COWI and PRC Bouwcentrum.
(with additional support from VEA) and the IWT O&O Project Tachwali, Y., Al-Assaf, Y., Al-Ali, A.R., 2007. Automatic multistage classification
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