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Waste Management 32 (2012) 869–878

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Waste Management
journal homepage: www.elsevier.com/locate/wasman

Washing of waste prior to landfilling


Raffaello Cossu, Tiziana Lai ⇑
University of Padua, IMAGE Department, Lungargine Rovetta, 8, I 35127 Padova, Italy

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

Article history: The main impact produced by landfills is represented by the release of leachate emissions. Waste wash-
Received 5 July 2011 ing treatment has been investigated to evaluate its efficiency in reducing the waste leaching fraction prior
Accepted 2 December 2011 to landfilling. The results of laboratory-scale washing tests applied to several significant residues from
Available online 15 January 2012
integrated management of solid waste are presented in this study, specifically: non-recyclable plastics
from source separation, mechanical–biological treated municipal solid waste and a special waste, auto-
Keywords: motive shredded residues. Results obtained demonstrate that washing treatment contributes towards
Waste washing
combating the environmental impacts of raw wastes. Accordingly, a leachate production model was
Sustainable landfilling
Final storage quality
applied, leading to the consideration that the concentrations of chemical oxygen demand (COD) and total
ASR, MBT Kjeldahl nitrogen (TKN), parameters of fundamental importance in the characterization of landfill leach-
Plastic sorting process residues ate, from a landfill containing washed wastes, are comparable to those that would only be reached
between 90 and 220 years later in the presence of raw wastes. The findings obtained demonstrated that
washing of waste may represent an effective means of reducing the leachable fraction resulting in a con-
sequent decrease in landfill emissions. Further studies on pilot scale are needed to assess the potential for
full-scale application of this treatment.
Ó 2012 Elsevier Ltd. All rights reserved.

1. Introduction wastes by rainwater, an interesting treatment option may be repre-


sented by the controlled washing of wastes prior to landfilling.
The sustainable landfill represents the most recent evolution in Numerous studies have demonstrated the efficacy of washing
the management of landfilled waste (Greedy, 2010; Scharff, 2006; of incineration residues in reducing the leachable fraction of
Hjelmar and Hansen, 2005). The design of a sustainable landfill is metals (Wang et al., 2001, 2009; Astrup, 2007; Van Herck and
based on a concept of multibarrier system: the latter foresees the Vandecasteele, 2001). Ishii et al. (2009) have developed, through
use of multiple barriers to produce a synergistic effect in reducing column tests, a model of use in establishing mechanisms to en-
the uncontrolled diffusion of leachate and biogas into the environ- hance removal of total organic carbon (TOC) from waste inciner-
ment. Accordingly, a decrease in waste quantities and the pre- ation residues.
treatment of landfilled wastes, final covering of the landfill and its Thus, the present paper reports the results of a study aimed to
ability to regulate leaching of wastes, control of biological degradation assess the effects produced by the washing of wastes performed
of deposited wastes, and the drainage and lining systems employed using two liquid/solid ratio (L/S) with different lengths of time.
in a landfill may all be considered barriers (Cossu, 1995). The differ- The study was carried out on two typical residues produced in the
ent methods of pre-treatment (mechanical–biological, thermal traditional management of municipal solid wastes (non-recyclable
treatment, etc.) and in situ treatment (forced aeration, semiaerobic plastics from source separation and mechanical–biological treated
landfill, flushing, etc.) should therefore be considered according to municipal solid waste) and on a special waste (automotive shredded
an integrated view (Stegmann et al., 2003). The aim is to develop residues). The disposal of the latter causes problems due to its com-
landfill sites capable of reducing environmental impacts over one plex matrix (Cossu and Gadia, 2007), particularly in the case of land-
generation to a level that no longer significantly affects the quality filling, the parameter to maintain under control is the dissolved
of the surrounding environment, whether air, water or soil. A similar organic carbon (DOC) content.
condition is habitually termed final storage quality (Cossu et al.,
2007; Baccini, 1989; Belevi and Baccini, 1989).
2. Materials and methods
In particular, as the main long-term impact produced by landfills
is represented by the emission of leachate from the leaching of
The scheme of the research is presented in Fig. 1.
Waste samples were washed on a laboratory scale; the effi-
⇑ Corresponding author. Tel.: +39 049 827 8990; fax: +39 049 827 8984. ciency of washing pre-treatment was evaluated by standard batch
E-mail addresses: tiziana.lai@unipd.it, lai.tiziana@gmail.com (T. Lai). leaching test to assess the improvement in landfill acceptability.

0956-053X/$ - see front matter Ó 2012 Elsevier Ltd. All rights reserved.
doi:10.1016/j.wasman.2011.12.005
870 R. Cossu, T. Lai / Waste Management 32 (2012) 869–878

the following parameters: DOC, COD, TKN and metals (As, Ba, Cd,
Cr, Cu, Hg, Mo, Ni, Pb, Se, Zn), chlorides, fluorides, and sulfates.
Methods applied in analyzing samples are reported in Table 1
(IRSA-CNR, 2003; US-EPA, 1996).

2.2. Laboratory-scale washing tests

Laboratory-scale washing tests were performed by placing


500 gTS of sample (ground to <4 mm) in an HDPE 5 l container,
and adding deionised water to reach L/S ratios of 5 and 10 l/kgTS.
The samples were continuously agitated by an overhead shaker
(Rotax 6.8) set at a speed of 20 rpm. Tests were conducted using
Fig. 1. Scheme of the experiment (L = amount of washing water, S = amount of treatment times of 3, 6, 12, 24 and 48 h.
washed waste, er = eluate of batch leaching test for the raw waste samples, Initially, tests were carried out considering only the parameter
ew = eluate of batch leaching test for the washed waste samples, Lr = leachate of DOC to determine the better conditions for washing among those
column test for the raw waste samples, Lw = leachate of column test for the washed
considered; from a sustainability point of view the best conditions
waste samples).
were defined by placing particular emphasis on duration of treat-
Leaching column tests were carried out on the waste to simulate ment and lowest efficient L/S ratios to be used in a potential
long-term emission potential on both raw and washed waste. full-scale application.
Washing conditions were selected on the basis of asymptotic
values obtained from elaboration of experimental DOC data using
2.1. Sample composition and characterization a desorption model based on a first order kinetic:

C ¼ C  ð1  ekt Þ ð1Þ
All experiments were performed on four different types of waste:
where, C = concentration of water solution substance (mg/l);
(a) undersieve residues from plastic sorting process (USP); C⁄ = equilibrium concentration (mg/l); k = rate constant (h1). Addi-
(b) end residues from plastic sorting process (ESP); tional parameters (TKN, COD, metals, chlorides, fluorides, sulfates)
(c) mechanical–biological treated waste (MBT); were analyzed in eluates corresponding to washing conditions
(d) automotive shredder residues (ASR). selected.

Samples (a) and (b) were collected in a sorting plant for source 2.3. Leaching column test
segregated plastics (Appendix A).
The USP residue was mainly constituted by non-recyclable fine Column tests were performed in glass columns (diameter 5 cm,
fraction (20% of the total input material), whilst the ESP residue height 30 cm). Leaching was obtained through introduction of
was made up of the non-recyclable heavy fraction (15% of the total deionised water by a peristaltic pump for low flow rates (model
input material). Watson Marlow 401D), from the bottom to the top of the column
Sample (c) was constituted by undifferentiated fraction of waste to avoid formation of unsaturated zones and preferential pathways
from separate collection after mechanical and biological treatment (CEN/292 method) as showed in Fig. 2. The flow rate was 0.012 l/h,
(4 weeks forced aeration and 6 weeks maturation phase). test duration was about 10 days.
All samples were collected in plants located in the Veneto The liquid released was collected to obtain a liquid–solid ratio
Region, Italy. The production of waste in the area per capita per of 1, 2, 5, 10 and 15 l/kgTS.
year is 475 kg. Source segregation rates are among the highest in Following filtration (10 lm), eluates were tested to determine
Italy (43%) (Regione Veneto, 2005). concentrations of the following parameters: pH, TKN, COD, TOC
Sample (d), collected from a shredder plant for end-of-life vehi- and metals.
cles (ELV), was constituted by non-recyclable fraction (approxi-
mately 25% of the total weight of ELV; Vermeulen et al., 2011). 3. Results and discussion
The plant is located in Northern Italy and produces approximately
6000 tons of ASR per year (2008). 3.1. Waste composition
All samples were collected according to the Italian reference
method UNI 10802 (2004). The findings obtained in composition of wastes studied are
The materials thus collected underwent classification in order summarized in Fig. 3.
to obtain a complete characterization of wastes. The materials The fine fraction (<20 mm) was increasingly present in waste
were separated into two fractions: fine fraction (<20 mm) and dif- samples subjected to grinding and/or sieving. This fraction is con-
ferent material fractions depending on the specific type of waste. sidered a separate category, as the small dimensions of the mate-
Prior to washing test all samples were ground to a size <4 mm rial did not allow additional classification. On the contrary, ESP
using a laboratory cutting mill (model Retsch SM 2000) and ana- sample included a large quantity of polymers exceeding 20 mm.
lyzed to determine both solid composition and leachable fraction
of waste by standard batch leaching test. 3.2. Waste characterization
The following parameters were analyzed on solid fractions:
total solids (TS), volatile solids (VS), seven day respirometric index The findings obtained for solid composition of wastes studied
(RI7), total Kjeldahl nitrogen (TKN), total organic carbon (TOC) and are illustrated in Table 2.
some metals (As, Ba, Cd, Cr, Cu, Hg, Mo, Ni, Pb, Se, Zn). The highest TOC content (63% TS) was obtained in the ESP sam-
Batch leaching tests, in accordance with standard UNI EN ple. The screened material, ASR and MBT featured TOC values rang-
12547-2, were performed using deionised water as extractant to ing between 33% and 40% TS.
obtain a liquid to solid ratio of 10 l/kgTS; the one step test has a Values revealed for seven day respirometric index (RI7) indi-
duration of 24 h. Eluates filtered at 0.45 lm were analyzed for cated a low biological activity for all materials.
R. Cossu, T. Lai / Waste Management 32 (2012) 869–878 871

Table 1
Reference analytical methods and equipment used in testing of liquid and solid samples.

Parameter Sample Reference method/equipment Description


TS Solid IRSA CNR Q.64/85 vol.2 n°2 Gravimetric methods after drying at 105 °C for 12 h
Liquid IRSA CNR 29/03 vol.1 n°2090 A
VS Solid IRSA CNR Q.64/85 vol.2 n°2 Gravimetric methods after drying at 550 °C for 4 h
RI7 Solid Sapromat and VoithSulzer Respiromat Static respirometric index
TKN Solid IRSA CNR Q.64/85 vol.3 n°6 Determination of ammonia by titration with a standard mineral acid, after
Liquid IRSA CNR 29/03 vol.2 n°5030 A conversion of amino nitrogen and free ammonia into ammonium by acid
digestion followed by distillation
TOC Solid Shimadzu TOC-VCSN analyzer Infrared detection of CO2 during dry combustion
Liquid Shimadzu TOC-VCSN analyzer
DOC Liquid IRSA CNR 29/03 vol.2 n°5040 Infrared detection of CO2 during dry combustion
COD Liquid IRSA CNR 29/03 vol.2 n°5130 Acid digestion with potassium dichromate followed by titration with Mohr’s salt
Ba, Cd, Cr, Cu, Mo, Ni, Pb, Zn Solid EPA 1996 n°6010 Analysis of aqua regia extracts by inductively coupled plasma
Liquid IRSA CNR 29/03 vol.1 n°3010+3020 atomic emission spectroscopy
As Solid EPA 1996 n°7061 Analysis of aqua regia extracts by atomic absorption spectrometry
Liquid IRSA CNR 29/03 vol.1 n°3010+3080A
Hg Solid EPA 1996 n°7471 Analysis of aqua regia extracts by atomic absorption spectrometry
Liquid IRSA CNR 29/03 vol.1 n°3010A+3200A2
Se Solid EPA 1996 n°7741 Analysis of aqua regia extracts by atomic absorption spectrometry
Liquid IRSA CNR 29/03 vol.1 n°3010A+3260A
Cl Liquid IRSA CNR 29/03 vol.2 n°4090 Direct titration with silver nitrate
F Liquid IRSA CNR 29/03 vol.2 n°4100B Potenziometric method
SO42 Liquid IRSA CNR 29/03 vol.2 n°4140A Turbidimetric method: precipitation of barium sulfate in HCl medium
pH Liquid IRSA CNR 29/03 vol.1 n°2060 Potentiometric method

The presence of nitrogen in wastes was mainly due to polyure-


thane plastics widely use for cars seats filling (Zia et al., 2007; Mar-
and et al., 2004), predominant in ASR, and to protein material and
humic substances, predominant in MBT (Tinter et al., 2010; Berthe
et al., 2008): the highest TKN content, corresponding to 1.3% TS,
was obtained for the ASR sample and for MBT (0.9% TS), whilst
the lowest value was observed in ESP sample (0.3% TS).
The highest quantities of metals were obtained for copper and
zinc. Concentrations determined in ASR sample were 7440 mg/
kgTS and 3820 mg/kgTS, respectively, corresponding to approxi-
mately 0.7% and 0.4% TS: this was due to the fact that copper
is present in electric wires whilst zinc is used as an additive in
tyres and paints. Copper and zinc concentrations exceeding
500 mg/kgTS were also obtained in USP and in MBT residues. In
the latter sample the presence of metals may have been caused
by wastes obtained from urban road dust, characterized by a sig-
nificant heavy metal content (Charlesworth et al., 2003; Wei and
Yang, 2010).
Results of batch leaching test are reported in Table 3.
On comparing the results obtained with those pertaining to so-
lid content, the nitrogen detected in the ASR sample was found to
be almost completely unleachable, being largely present as a com-
ponent of polyurethane plastics.
Moreover, in USP and ESP samples significant amounts of leach-
able fraction of nickel and zinc, higher than 20% and 5%, respec-
tively, were also detected.

3.3. Laboratory-scale washing test

3.3.1. Test results and modeling


The results of washing tests illustrated in Table 4 report an Fig. 2. Leaching column test apparatus.
increasing DOC trend (expressed as mgC/kgTS) associated to both
duration of treatment and L/S ratios used in washing. Asymptotic values were similar to those obtained in standard
The desorption model applied interpolated in a satisfactory batch leaching tests for USP, ESP and MBT, slightly lower in the
manner with DOC concentrations measured in washing eluates case of L/S of 5 l/kgTS and without significant differences in the case
on varying duration of treatment to correspond to a specific L/S of L/S of 10 l/kgTS; only in the case of ASR sample were values
ratio: values obtained for Mean Absolute Percent Error (MAPE) were calculated by the model lower than those obtained in standard
within the range of 2  10%. batch leaching tests (Table 5).
Fig. 4 illustrates an example of the curve obtained following The L/S ratio to be applied in a potential full-scale washing of
application of the desorption model to DOC values measured in wastes was determined by comparing asymptotic DOC values
eluates from tests performed on wastes at an L/S ratio of 5 l/kgTS. established by the desorption model.
872 R. Cossu, T. Lai / Waste Management 32 (2012) 869–878

Fig. 3. Composition of raw waste samples.

Table 2 Table 4
Chemical–physical composition of solid matrix in wastes investigated. DOC released amounts expressed as mg/kgTS measured in eluates at the end of
washing tests associated to duration (h) and L/S ratio (l/kgTS).
USP ESP MBT ASR
Time (h) L/S
TS gTS/gRW 0.79 0.98 0.81 0.85
VS gVS/gTS 0.59 0.89 0.48 0.51 USP ESP MBT ASR
RI7 gO2/kgTS 3.8 2.0 2.2 3.0
5 10 5 10 5 10 5 10
TOC gC/kgTS 400 630 380 330
TKN mgN/kgTS 8000 3100 8800 12,900 3 7700 7660 3645 4030 4825 5270 349 485
As mg/kgTS n.d. 0.05 0.08 0.16 6 8980 9080 4415 4860 5690 5870 480 594
Ba mg/kgTS 11.9 9.8 7.8 12.8 12 9945 9220 5240 6090 6230 6480 487 505
Cd mg/kgTS 1.33 n.d. 0.5 11.8 24 8040 7840 5595 6420 6560 6480 488 671
Cr mg/kgTS 15.7 4.1 79 117 48 9395 9620 5710 7820 6190 6940 637 747
Cu mg/kgTS 1388 22 583 7443
Hg mg/kgTS 4.3 1.2 2.32 0.12 USP = under-sieve residues from plastic sorting process, ESP = end residues from
Mo mg/kgTS 1.79 1.09 2.4 19.3 plastic sorting process, MBT = mechanical–biological treated waste, ASR = auto-
Ni mg/kgTS 13.8 2.5 16 346 motive shredder residues.
Pb mg/kgTS 215 8.2 131 409
Se mg/kgTS n.d. n.d. 0.11 n.d.
Zn mg/kgTS 554 120 452 3815 The latter clearly underlines how washing tests for this type of
waste should be performed at an L/S ratio of 5 l/kgTS. Likewise,
USP = under-sieve residues from plastic sorting process, ESP = end residues from
the same ratio should be applied in washing of ESP and of MBT
plastic sorting process, MBT = mechanical–biological treated waste, ASR = auto-
motive shredder residues. samples. Moreover, following washing at a ratio of 5, approxi-
n.d. = Value under instrument detection limit. mately 73% of the leachable content of ASR sample is eliminated
using an L/S ratio of 10 l/kgTS: to obtain an approximately 27% in-
crease in removal the quantity of water would have to be increased
With regard to the USP sample, the results obtained emphasize 100%. In view of a possible full-scale application, the marked water
how washing at an L/S of 5 l/kgTS would enhance leaching of 98% consumption required at a high L/S ratio would however result in
the amount that could be desorbed at an L/S ratio of 10 l/kgTS. an L/S ratio of 5 being considered feasible.

Table 3
Released amount (mg/kgTS) compared with concentration in solid (%) of parameters measured in eluates from batch leaching tests on raw waste samples.

USP ESP MBT ASR


(mg/kgTS) (%) (mg/kgTS) (%) (mg/kgTS) (%) (mg/kgTS) (%)
DOC 10,070 2.5 6470 1 6870 1.8 1020 0.3
TKN 850 11 580 19 870 9.9 80 0.6
Ba 3 25 1 10 1 13 1.5 12
Cr 0.3 1.9 0.2 4.9 2 2.5 n.d. n.d.
Cu 3 0.2 0.4 1.8 12 2.1 2 0
Mo 0.3 17 0.4 37 1.1 46 0.5 2.6
Ni 3.1 22 0.5 20 3.3 20 0.2 0.1
Pb 1.4 0.7 n.d. n.d. 0.9 0.7 n.d. n.d.
Zn 34 6.1 6 5.0 12 2.7 1 0

USP = under-sieve residues from plastic sorting process, ESP = end residues from plastic sorting process, MBT = mechanical–biological treated waste, ASR = automotive
shredder residues.
n.d. = Value under instruments detection limit (As, Cd, Hg, Se are non-reported because under instrument detection limit for all samples).
R. Cossu, T. Lai / Waste Management 32 (2012) 869–878 873

Fig. 4. Desorption model application of DOC concentration values measured in eluates of washing with L/S = 5 l/kgTS.

Table 5
Asymptotic values of DOC released amounts (C⁄) calculated through application of a
dynamic desorption model to results obtained in washing tests carried out at an L/S
ratio of 5 and 10 l/kgTS. Results obtained from standard leaching batch test are also
reported (C).

C k5 C ⁄5 k10 C⁄10 C⁄5/C⁄10


(mgC/kgTS) (h1) (mgC/kgTS) (h1) (mgC/kgTS) (%)
USP 10,070 0.57 9395 0.53 9620 98
ESP 6470 0.35 5600 0.33 6430 87
MBT 6870 0.50 6200 0.56 6480 96
ASR 1020 0.42 490 0.42 670 73

USP = under-sieve residues from plastic sorting process, ESP = end residue from Fig. 5. Percentage of DOC removed through the application of desorption model
plastic sorting process, MBT = mechanical–biological treated waste, ASR = auto- starting from values measured in washing eluates (L/S = 5 l/kgTS) of wastes. Curves
motive shredder residues. were normalized with respect to the asymptotic value obtained by the model. The
broken line indicates the 6 h washing duration.

The duration of washing was determined on the basis of time Table 6


trends obtained through application of the model to washing tests Concentration of different substances measured in residual water resulting from the
washing test (t = 6 h, L/S = 5 l/kgTS), compared with limit values established by Italian
conducted at an L/S of 5 l/kgTS (Fig. 5). law (D.M. 152/2006) for discharge into the domestic sewerage system.
In all samples investigated, a 6-h washing treatment led to
removal of more than 85% of asymptotic DOC concentration (i.e. USP ESP MBT ASR Discharged limits

the maximum removable amount) calculated by the model. In TOC mgC/l 1796 883 1138 96 –
the case of USP, the removal obtained exceeded 95%. In the light COD mgO2 =l 3303 3846 3555 208 6500
TKN mgN/l 258 149 190 n.d. 630 (as ammoniac nitrogen)
of these results a 6-h period was identified as the better washing
Ba mg/l 0.08 0.17 0.09 0.11 –
duration among those tested. Cd mg/l n.d. n.d. n.d. 0.02 60.02
For full scale applications of waste washing further research is Cr mg/l 0.03 0.03 0.20 n.d. 64
required in order to optimize the L/S ratio and the most appropri- Cu mg/l 0.11 0.04 0.81 0.15 60.4
ate operative conditions (water recirculation, drying before land- Mo mg/l 0.04 0.06 0.07 0.07 –
Ni mg/l 0.41 0.06 0.35 0.03 64
filling, etc.), and to assess the energetic and economic balance. Pb mg/l 0.12 n.d. 0.09 n.d. 60.3
Zn mg/l 1.37 1.31 0.81 0.07 61.0
3.3.2. Characterization of residual water resulting from washing tests USP = under-sieve residues from plastic sorting process, ESP = end residues from
(L/S = 5 l/kgTS, t = 6 h) plastic sorting process, MBT = mechanical–biological treated waste, ASR = auto-
Table 6 illustrates the concentration of different substances in motive shredder residues.
the residual water resulting from the washing test at L/S of 5 l/kgTS n.d. = Value under instruments detection limit (As, Cd, Hg, Se are non-reported
because under instrument detection limit for all samples).
and 6-h duration. This residual water should be treated in a
wastewater treatment facility, with the exception of residual
water from ASR washing which can be directly discharged into
the domestic sewerage system, as established by Italian law 3.3.3. Washing efficiency and landfill acceptability
(D.M. 152/2006). The concentrations obtained for parameters measured in batch
The results obtained, expressed in terms of amounts released leaching tests carried out on the four raw waste samples (er)
(Table 7), demonstrate how the washing test at L/S of 5 l/kgTS studied are reported in Table 8. The measured values were com-
and 6-h duration allows a large part of the leachable waste fraction pared with limits established by Italian regulations (D.M. 27/09/
to be removed (Table 3). In particular, values of TOC and TKN re- 2010) for waste acceptance in landfill.
moved were in line with those obtained from batch leaching test DOC concentrations obtained in eluates from all raw wastes
and confirmed by values obtained for improvement of landfill studied exceeded limits established for disposal in hazardous
acceptability illustrated in Table 8. waste landfills. However, in accordance with Italian legislation
874 R. Cossu, T. Lai / Waste Management 32 (2012) 869–878

Table 7 conditions selected (L/S = 5 l/kgTS, t = 6 h), according to the follow-


Released amount (mg/kgTS) of parameters measured in the residual water resulting ing equation:
from washing test (t = 6 h, L/S = 5 l/kgTS).

USP ESP MBT ASR


gA;i ¼ ðer;i  ew;i Þ=er;i ð2Þ

TOC mgC/kgTS 8980 4415 5690 480 where, er,i = concentration of the i-substance in the eluate of batch
TKN mgN/kgTS 1290 745 950 n.d. leaching test for raw waste; ew,i = concentration of the i-substance
Ba mg/kgTS 0.40 0.85 0.45 0.55
in the eluate of batch leaching test for washed waste.
Cd mg/kgTS n.d. n.d. n.d. 0.10
Cr mg/kgTS 0.15 0.15 1.00 n.d. Concentrations detected in eluates and washing efficiency (gA,i)
Cu mg/kgTS 0.55 0.20 4.05 0.75 after waste washing treatment, for more significant parameters
Mo mg/kgTS 0.20 0.30 0.35 0.35 analyzed, are shown in Table 8.
Ni mg/kgTS 2.05 0.30 1.75 0.15 Removal efficiency for TKN was particularly significant: for the
Pb mg/kgTS 0.60 n.d. 0.45 n.d.
Zn mg/kgTS 6.85 6.55 4.05 0.35
USP sample the concentration of this parameter present in eluates
from batch leaching tests was decreased by 76% following treat-
USP = under-sieve residues from plastic sorting process, ESP = end residues from ment, from a value of 85 mgN/l to a value of 20 mgN/l.
plastic sorting process, MBT = mechanical–biological treated waste, ASR = auto-
DOC removal efficiency ranged from 22% for MBT and 85% for
motive shredder residues.
n.d. = Value under instruments detection limit (As, Hg, Se are non-reported because USP samples. DOC removal revealed for ASR waste reached 53%,
under instrument detection limit for all samples). with a decrease of concentration in eluates from batch leaching
tests from an initial 102 mg/l to 48 mg/l after washing. A similar
decrease would be sufficient to allow the disposal of ASR in a land-
(D.M. 27/09/2010), this parameter is important for assessing land- fill for inert wastes.
fill acceptability exclusively for residues different from municipal Removal percentages obtained for COD are comparable to those
solid wastes (MSW). Therefore, among the waste taken into con- obtained for DOC.
sideration, it applies only to ASR residue and not to the other With regard to the heavy metal content, in all samples investi-
wastes examined which could be considered similar to MSW for gated copper and zinc concentrations in eluates obtained from
quality and quantity. batch leaching tests following washing were significantly lower
The highest COD values (approximately 2590 mgO2 =l) were ob- (a decrease of approximately 90%). Removal percentages for other
tained in eluate from the USP sample, whilst the lowest concentra- metals analyzed varied according to type of waste: e.g. the removal
tions, approximately 240 mgO2 =l, were obtained for ASR residues. efficiency for nickel ranged from 32% (ESP) and 73% (MBT).
TKN content was higher in eluates from MBT residues (87 mgN/l),
whilst lower concentrations were observed in ASR eluate (8 mgN/l). 3.4. Long-term emission potential of washed waste
With regard to metals, the highest concentrations were
detected for copper (0.3 mg/l in eluate from USP and 1.2 mg/l in The long-term pollution potential of a landfill is determined by
eluate from MBT) and zinc (3.4 mg/l in eluate from USP and the residual concentrations of compounds present in leachate. The
1.2 mg/l in eluate from MBT). In eluates from USP and from MBT longest lasting environmental impacts of a landfill are caused by
residues, nickel concentrations of 0.31 and 0.33 mg/l were ob- the presence of ammonia nitrogen in leachate (Kjeldsen et al.,
tained. Metal concentrations measured in ASR eluate were gener- 2002). Furthermore, several studies on municipal solid waste have
ally low and complied with limits established for landfill disposal demonstrated that metals reach environmentally sustainable
of inert wastes. concentrations in leachate over long periods (Revans et al.,
The highest concentrations of chlorides and sulfates, 535 and 1999); although pre-treatment of waste (e.g. composting) seems
559 mg/l, respectively, were detected in eluate from MBT residues. to reduce the mobility of metals such as nickel, lead and zinc
Washing efficiency, from the point of view of improvement of (van Praagh et al., 2009).
landfill acceptability, was determined by calculating removal of Leaching column tests were carried out on the waste to simu-
the leachable component of waste obtained by applying washing late long-term emission potential on both raw and washed waste

Table 8
Batch leaching test results before (er) and after treatment (ew), and washing efficiency (gA,i). Concentrations in eluates are compared to limits established by Italian regulation
(D.M. 27/09/2010) for waste acceptance in landfill (I = inert, NH = non-hazardous, SH = stable non-reactive hazardous, H = hazardous).

USP ESP MBT ASR Landfilling limits


er ew lA,i er ew lA,i er ew lA,i er ew lA,i I NH SH H
(mg/l) (mg/l) (%) (mg/l) (mg/l) (%) (mg/l) (mg/l) (%) (mg/l) (mg/l) (%) (mg/l) (mg/l) (mg/l) (mg/l)
DOC 1007 155 85 647 280 57 687 539 22 102 48 53 50 100 80 100
COD 2592 385 85 2105 950 55 1997 1050 47 237 70 70 – – – –
TKN 85 20 76 58 29 50 87 29 67 8 <5 >38 – – – –
Ba 0.3 0.09 74 0.1 0.04 22 0.1 0.1 0 0.15 0.11 28 2 10 10 30
Cr 0.03 <0.01 >67 0.02 <0.01 >50 0.2 0.05 76 <0.01 <0.01 n.c. 0.05 1 1 7
Cu 0.3 0.03 89 0.04 0.01 73 1.2 0.03 97 0.2 0.02 87 0.2 5 5 10
Mo 0.03 0.02 37 0.04 0.03 28 0.11 0.04 64 0.05 0.04 35 0.05 1 1 3
Ni 0.31 0.10 67 0.05 0.03 32 0.33 0.09 73 0.02 <0.02 0 0.04 1 1 4
Pb 0.14 0.09 33 <0.03 <0.03 n.c. 0.09 0.06 28 <0.03 <0.03 n.c. 0.05 1 1 5
Zn 3.4 0.32 91 0.6 0.07 89 1.2 0.13 89 0.1 0.02 88 0.4 5 5 20
Cl 369 92 75 291 121 59 535 213 60 71 28 60 80 2500 1500 2500
F 0.3 0.2 33 0.2 0.2 0 0.4 0.3 25 0.6 0.4 33 1 15 15 50
SO42 205 70 66 117 47 60 559 137 75 27 22 17 100 5000 2000 5000
pH 7.5 7.4 – 7.4 7.5 – 7.4 7.4 – 7.7 7.5 – – – – –

USP = under-sieve residues from plastic sorting process, ESP = end residues from plastic sorting process, MBT = mechanical–biological treated waste, ASR = automotive
shredder residues.
As, Cd, Hg, Se are non-reported as under instrument detection limit for all samples.
n.c. = Values measured in eluates of raw waste were lower than instrument detection limit.
R. Cossu, T. Lai / Waste Management 32 (2012) 869–878 875

Table 9
Cumulative concentrations of parameters analyzed in eluates from column leaching tests on raw waste samples (Lr) and washed waste samples (Lw).

USP ESP MBT ASR


L/S 1 2 5 10 15 1 2 5 10 15 1 2 5 10 15 1 2 5 10 15
TOC Lr gC/kgTS 0.95 2.46 4.88 6.65 7.97 0.33 0.98 2.31 4.44 6.80 0.93 2.79 5.41 8.34 10.5 0.14 0.39 0.79 1.15 1.51
Lw 0.52 1.20 2.22 3.84 5.34 0.27 0.71 1.63 2.99 4.43 1.44 3.58 8.07 12.7 15.5 0.09 0.25 0.52 0.84 1.25
COD Lr gO2/kgTS 3.13 9.29 19.8 28.0 34.2 2.61 6.97 14.7 23.1 35.1 4.41 12.5 25.4 40.8 55.7 0.31 0.93 1.68 2.34 2.81
Lw 1.35 3.65 5.98 8.43 11.6 0.90 2.51 5.61 8.04 11.7 3.65 8.75 16.8 23.5 32.6 0.15 0.36 0.61 1.06 1.51
TKN Lr gN/kgTS 0.21 0.56 1.12 1.53 1.71 0.06 0.17 0.40 0.66 0.91 0.25 0.72 1.35 2.13 2.66 – – – – –
Lw 0.05 0.14 0.25 0.36 0.46 0.04 0.12 0.24 0.39 0.54 0.10 0.25 0.54 0.82 1.04 – – – – –
Ba Lr mg/kgTS 0.11 0.23 0.78 1.48 2.23 – – 0.50 1.50 2.85 0.06 0.17 0.38 0.78 1.08 0.54 1.12 1.77 2.87 4.22
Lw 0.09 0.27 0.67 1.17 2.07 – – 0.45 1.15 2.20 0.31 0.63 1.33 1.73 2.18 0.29 0.67 1.52 3.02 4.82
Cr Lr mg/kgTS 0.04 0.12 0.22 0.32 0.32 – – 0.10 0.20 0.35 0.27 0.75 1.60 2.80 3.55 – – – – –
Lw 0.02 0.04 0.09 0.09 0.09 – – – – – 0.11 0.31 0.71 1.11 1.41 – – – – –
Cu Lr mg/kgTS 0.26 0.64 1.39 2.49 2.64 – – 0.45 0.85 1.30 1.86 4.88 8.23 12.3 15.6 0.08 0.24 0.49 0.79 1.09
Lw 0.16 0.34 0.74 1.34 1.64 – – 0.10 0.40 0.70 0.11 0.27 0.67 1.57 2.02 0.05 0.13 0.28 0.48 0.78
Mo Lr mg/kgTS 0.06 0.14 0.24 0.34 0.34 – – 0.20 0.40 0.55 0.15 0.43 0.83 1.33 2.08 0.09 0.25 0.65 1.45 1.60
Lw 0.03 0.07 0.12 0.22 0.22 – – 0.15 0.35 0.50 0.04 0.08 0.18 0.18 0.18 0.08 0.22 0.57 1.07 1.67
Ni Lr mg/kgTS 0.65 1.71 3.41 4.91 5.81 – – 0.25 0.45 0.60 0.51 1.39 2.89 4.79 5.69 0.03 0.09 0.19 0.39 0.54
Lw 0.22 0.56 1.06 1.66 2.11 – – 0.10 0.20 0.50 0.14 0.36 0.81 1.21 1.51 0.02 0.04 0.09 0.09 0.09
Pb Lr mg/kgTS 0.15 0.33 0.58 0.88 0.88 – – – – – 0.14 0.40 1.00 2.00 3.35 – – – – –
Lw 0.11 0.23 0.48 0.48 0.48 – – – – – 0.11 0.29 0.74 1.44 2.34 – – – – –
Zn Lr mg/kgTS 1.71 3.31 5.86 12.4 15.2 – – 3.10 6.50 9.95 2.02 3.86 6.21 9.21 12.5 0.06 0.12 0.27 0.47 0.62
Lw 0.48 0.94 1.79 3.19 4.99 – – 0.30 1.00 1.45 0.19 0.45 1.00 2.10 3.00 0.04 0.08 0.18 0.28 0.43
pH Lr – 7.6 7.9 7.4 7.1 6.7 7.4 7.6 7.4 7.0 7.0 6.9 7.5 7.6 7.5 7.3 7.6 8.1 8.0 8.0 7.8
Lw 7.6 7.4 7.3 7.2 7.2 7.7 7.6 7.3 7.4 7.0 7.3 7.5 7.5 7.3 7.4 7.9 8.0 7.9 7.8 7.4

USP = under-sieve residues from plastic sorting process, ESP = end residues from plastic sorting process, MBT = mechanical–biological treated waste, ASR = automotive
shredder residues.
As, Cd, Hg, Se are non-reported as under instrument detection limit for all samples.

Fig. 6. Values of COD obtained by applying the model for prevision of landfill long-term emissions to concentrations assayed in eluates from column tests of raw and washed
waste (L/S = 5 l/kgTS; t = 6 h). The hatched part of the graph corresponds with the opening period of the landfill; the broken line corresponds to the end of the financial
guarantee period (30 years after closure).

(Table 9). Cumulative concentrations of parameters analyzed in in leachate following landfilling of raw and washed wastes,
eluates from washed waste sample were generally lower than elu- respectively.
ates from raw samples, with the exception of TOC, and to a lesser To this regard, a hypothetical landfill with a surface area of
extent, barium, in the case of MBT; this is probably due to the het- 13 hectares and an average height of 10 m was taken into consider-
erogeneity of the sample. ation. The operational phase during which wastes are conferred was
The effects of waste washing on long-term impacts was taken as 10 years (1 sector with 1.3 hectares of surface per year).
evaluated by comparing, in particular, the potential time The cumulative leachate production was estimated using a mod-
trends obtained for COD and TKN concentrations registered el based on mass balance of water influx and water released from
876 R. Cossu, T. Lai / Waste Management 32 (2012) 869–878

Fig. 7. Values of TKN obtained by applying the model for prevision of landfill long-term emissions to concentrations assayed in eluates from column tests of raw and washed
waste (L/S = 5 l/kgTS; t = 6 h). The hatched part of the graph corresponds with the opening period of the landfill; the broken line corresponds to the end of the financial
guarantee period (30 years after closure).

each sector of the landfill (Canziani and Cossu, 1989; Cossu et al., The estimates obtained by the model should be considered whilst
1988), considering a waste density of 0.7 t/m3and an absorption taking into account that column test conditions are not entirely com-
capacity of 0.16 m3/t (Blakey, 1992), in the presence of a cover of parable to those present in a landfill (Heyer and Stegmann, 1997). In
clayey soil in the cultivation period and a planted soil cover after particular, waste composition is not homogeneous and the organic
landfill closure. Rainfall was taken as mean monthly amounts matter present could reach different degree of degradation that
registered in the Veneto region from 1994 to 2007 and was equal influence the mobilization potential of contaminants (Andreottola
to 1040 mm/y (ARPAV, 2008). and Cannas, 1992). Furthermore percolation through the landfill
The correspondence between L/S evaluated in column leaching body varies, and contact times between water and waste may differ
test, 1, 2, 5, 10, 15 l/kgTS, and the time required to reach the same as in presence of preferential flow pathways, as a consequence leach-
L/S ratio for the hypothetical landfill was 25, 43, 98, 190 and ate quality could reflect processes within waste mass in the sur-
280 years, respectively. roundings of preferential flow paths and not in the whole landfill
The time trend observed for COD and TKN concentrations in systems (Fellner et al., 2009; Rosqvist et al., 2005; Rosqvist and Des-
leachate was established by interpolating concentrations mea- touni, 2000).
sured in eluates from column leaching tests and following washing Time trends relating to COD and TKN, obtained by applying the
(L/S = 5 l/kgTS, t = 6 h) according to the following formula (Belevi model for prevision of long-term emissions to concentrations
and Baccini, 1989; Heyer and Stegmann, 1997): assayed in eluates from column tests carried out on the wastes
investigated before and after washing treatment (L/S = 5 l/kgTS,
C t ¼ C 0  ekðtT 0 Þ ð3Þ
t = 6 h) are represented in Figs. 6 and 7.
where, Ct = concentration of substance determined at time t (mg/l); To verify the efficacy of washing treatment in achieving envi-
C0 = concentration of substance determined at time T0 (mg/l); ronmental sustainability of a landfill, COD and TKN concentra-
k = indicative velocity coefficient for decreasing concentration over tions estimated by the model at the end of the financial
time (y1); T0 = time taken as start of model simulation. As a general guarantee period, were assessed. The period established by law
rule the time coincides with the duration of reaction time initially for financial provisions (D.Lgs. 36/2003) is of 30 years after land-
occurring within the landfilled wastes; in the present case this per- fill closure.
iod was hypothesized to last throughout the entire length of landfill All waste samples evaluated to assess the time trend of COD
operations (10 years). concentration in leachate through application of the model dis-
The hypotheses underlying the application of the model con- played lower concentrations for washed wastes.
cerned are as follows: With regard to USP sample, it was observed how 30 years after
landfill closure leachate from washed wastes features a COD con-
– constant factors influencing leaching of substances from land- centration that would only have been achieved 130 years later if
filled wastes (pH, redox conditions, etc.) over time; wastes had not been washed (Fig. 6).
– the main factor involved in emission abatement if leaching pro- A similar observation was made for simulations carried out
duced by rainwaters; using the remaining samples investigated: at the end of the finan-
– the time-related decrease in concentrations of substances pres- cial guarantee period leachate obtained from washed ASR was
ent in leachate can be described by means of a first order characterized by concentrations similar to those that would be
kinetic. obtained for raw wastes only 120 years after landfill closure.
R. Cossu, T. Lai / Waste Management 32 (2012) 869–878 877

Fig. 7 illustrates the trends obtained for TKN. The curve ob- ily leachable fraction, but may not significantly affect the emission
tained for ASR is not illustrated as TKN concentrations measured potentials associated with mobilization processes occurring at a
in eluates from column leaching tests were below detection limits slower rate from the deposited waste.
(<5 mg/l). For full scale applications of waste washing further research is
Similar to the trend observed for COD, the time trend of TKN needed in order to evaluate the influence of the waste grain size,
concentration in leachate as simulated by the model were de- optimize the L/S ratio and the most appropriate operative condi-
creased following washing procedures performed under L/S = 5 l/ tions (water recirculation, drying before landfilling, etc.), and to
kgTS and t = 6 h conditions. assess the energetic and economic balance.
With regard to USP, thirty years after landfill closure leachate
from washed wastes features TKN concentrations that would nor-
Acknowledgments
mally only be reached after a period of 160 years in the presence of
raw wastes. Similar results also applies to MBT residues.
The authors wish to express their appreciation for her precious
Significant findings have been determined for ESP: leachate ob-
support to Dr. Annalisa Sandon Head of the Analytical Laboratory
tained from washed wastes presented concentrations that would
of Sanitary Engineering and Environmental (LISA) of the University
otherwise have been achieved with raw wastes only after a period
of Padua, and wish to thank Bruno Sartorello for taking part in the
of 90 years subsequent to landfill closure.
experimental work.
The grain size of waste, of course, is a factor which may influence
the efficiency of washing at full-scale applications. This aspect will
be evaluated in future research. However the grain size considered Appendix A. Supplementary data
in the present experiment can accurately represent waste display-
ing a prevalence of fine fraction (USP, MBT, ASR). Supplementary data associated with this article can be found, in
the online version, at doi:10.1016/j.wasman.2011.12.005.

4. Conclusions
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