Waste Management 118 (2020) 68–78

Contents lists available at ScienceDirect

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

Environmental life cycle assessment of the recycling processes of waste

plastics recovered by landfill mining
Grazia Maria Cappucci a,b,1, Roberto Avolio c,1, Cosimo Carfagna c, Mariacristina Cocca c, Gennaro Gentile c,
Simone Scarpellini a,b, Francesco Spina d, Gianluigi Tealdo d, Maria Emanuela Errico c,⇑,
Anna Maria Ferrari a,b,⇑
a
Department of Sciences and Methods for Engineering, University of Modena and Reggio Emilia, Reggio Emilia, Piazzale Europa 1, 42122 Reggio Emilia, Italy
b
EN&TECH, Interdepartmental Research Centre for Industrial Research and Technology Transfer in the field of Integrated Technologies for Sustainable Research,
Efficient Energy Conversion, Building Energy Efficiency, Lighting and Home Automation, Reggio Emilia, Piazzale Europa 1, 42122, Italy
c
Institute for Polymers, Composites and Biomaterials, National Research Council of Italy(IPCB-CNR), via Campi Flegrei 34, 80078 Pozzuoli, Italy
d
IREOS S.p.A., via Stefano Turr 165, 16147 Genova, Italy

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

Article history: Enhanced Landfill Mining (ELFM) is a powerful tool for the sustainable management of landfill sites, aim-
Received 22 April 2020 ing at both land reclamation and material recovery/reuse. To enhance the recovery and recycling rate of
Revised 26 June 2020 excavated plastic fractions, in most cases destined to energy recovery, new convenient, effective and sus-
Accepted 28 July 2020
tainable strategies are needed. In this study, a recovery and valorization process of ELFM excavated plas-
Available online 2 September 2020
tics has been validated through an integrated experimental and Life Cycle Assessment (LCA) approach,
demonstrating the environmental sustainability of the secondary raw material generated, in terms of
Keywords:
use of resources and emissions generated. In particular, the secondary granulate from ELFM was com-
Landfill mining
Life cycle assessment
pared with a virgin product and the last one resulted to have a higher impact (more than 4.46 times
Waste recovery greater than the first one), in particular for the use of the resource crude oil as raw material in the pro-
Circular economy duction of primary LDPE. The valorization process of the excavated plastic made the mechanical proper-
ties of the secondary raw material comparable to that of a primary material.
Ó 2020 Elsevier Ltd. All rights reserved.

1. Introduction
The management of landfill sites is a pressing issue for the
countries of the EU area. Advanced waste management policies
and directives are pointing towards a ‘‘zero waste” goal; however,
disposal by landfilling is still diffused and over 500 000 landfills
have been reported in the EU, of which 90% operated before the
introduction of specific directives (1999/31/EC) and thus poten-
Abbreviations: ATR, total reflectance accessory; EDX, energy dispersive X-ray
analysis; ELFM, enhanced landfill mining; GWP, global warming potential; HEPA,
high efficiency particulate air filters; LCA, life cycle assessment; LCI, life cycle
inventory; LDPE, low density polyethylene; LFM, landfill mining; LLDPE, linear low
density polyethylene; MAPE, maleated linear low density polyethylene; MIBC,
methyl-isobutyl-carbinol; PE, polyethylene; PET, polyethylene terephthalate; PP,
polypropylene; PS, polystyrene; Pt, point; PVC, polyvinyl chloride; RDF, waste-
derived fuels; SEM, scanning electron microscopy; TGA, thermogravimetric anal-
ysis; WP, waste plastic.
⇑ Corresponding authors.
E-mail addresses: mariaemanuela.errico@ipcb.cnr.it (M.E. Errico), annamaria.
ferrari@unimore.it (A.M. Ferrari).
1
Both authors contributed equally to this work.
tially unsafe. Landfill sanitation and reclamation activities are then
increasingly implemented by public institutions. The increased
sensitivity for a sustainabile life cycle of products and materials,
exemplified by the circular economy concept, has recently led to
a new paradigm in waste management, where waste-derived sec-
ondary raw materials can be introduced in the production cycles.
In this frame, landfills should be viewed as ‘‘mines” of raw
resources to be extracted and valorized. Landfill mining (LFM)
operations are based on the excavation, separation and appropriate
re-treatment of wastes with the double aim of 1) land reclamation/
environmental remediation of landfill sites and 2) materials recov-
ery and recycling, with environmental and economic benefits
(Jones et al., 2013). The maximization of land and raw materials
recovery requires innovative technologies and an integrated
approach (Enhanced Landfill Mining, ELFM), whose implementa-
tion must be guided by a systematic and comprehensive analysis
of the environmental benefits and burden associated.
LFM and ELFM were analysed from an environmental point of
view through Life Cycle Assessment methodology by several
authors. The LFM applied to a non-controlled municipal landfill

https://doi.org/10.1016/j.wasman.2020.07.048
0956-053X/Ó 2020 Elsevier Ltd. All rights reserved.
 G.M. Cappucci et al. / Waste Management 118 (2020) 68–78
in the U.S.A. was studied by Jain and colleagues (Jain et al., 2014),
with three hypothetical scenarios: the excavation of waste fol-
lowed by recovery of material and energy was compared with
excavation and re-burial of waste in a properly managed landfill
and with a ‘‘Do-nothing” scenario, in which the landfill is not sub-
ject to mining operations. Significant differences in the environ-
mental damage between the above mentioned scenarios were
assessed for some categories identified in the EDIP 97 method
(Wenzel et al., 1997), in particular global warming potential
(GWP), acidification, human toxicity via soil and human toxicity
via surface water. In these categories, the first scenario benefited
from environmental advantages, thanks to the recovery of metals
and the replacement of coal for energy production, while the third
scenario showed the greatest impact, due to the methane emis-
sions produced by the decomposition of the waste and no environ-
mental advantage in any other categories. The disadvantages of a
do-nothing approach were also underlined by Danthurebandara
and colleagues (Danthurebandara et al., 2014), who studied the
ELFM process operated on a Belgian municipal and industrial land-
fill where the treatment process was supported by biogas and lea-
chate collection and treatment operations.
The impact of logistics on ELFM sustainability was observed by
Gusca and colleagues (Gusca et al., 2015) analyzing two LFM alter-
natives applied to the Riga landfill. Through IMPACT 2002+ evalua-
tion method (Jolliet et al., 2003) the greatest contributions to the
total impact were represented by the processes of excavation and
transport due to fuel consumption, so that the use of an on site
treatment plant with mobile machines led to a 28% reduction in
impact with respect to a stable ex-situ plant.
Finally, it is reported that within ELFM, recycling is often lim-
ited to metals, glass and aggregates, while materials such as wood,
textiles, paper and, notably, plastics, are usually converted to
waste-derived fuels (RDF) (Canopoli et al., 2018). Plastics, in partic-
ular, are found as a major component in most landfills ((Kaartinen
et al., 2013); (Canopoli et al., 2018); (Pecorini and Iannelli, 2020)).
A large abundance of polyolefin materials (PE, PP) can be generally
expected in excavated plastics, but variable amounts of other com-
mon polymers (PET, PVC, PS) are usually present ((Schwarzböck
et al., 2017); (Zhou et al., 2014)). The energy recovery approach
is not exempt from environmental problems: the damage analysis
conducted with the end-point ReCiPe method by Goedkoop et al.
(2013), showed that the plasma gasification process of ELFM recov-
ered organic fractions caused the largest contribution to total dam-
age, in particular in the climate change category. Nevertheless,
alternative approaches as the recycling of excavated plastics as
secondary raw materials have been hindered by the need to sepa-
rate the different polymers present and by the need to cope with
unavoidable contaminations (soil matter, organic leachates but
also harmful substances such as heavy metals, (Wolfsberger
et al., 2015)) and degradation induced by the landfilling conditions.
Recently, an effective separation of plastic fractions has been
obtained by combination of appropriate pretreatment and near
infrared (NIR) sensor based sorting (Küppers et al., 2019).
In this paper, the experimental feasibility of valorization and
recycling of an ELFM recovered plastic fraction was demostrated
and the environmental sustainability of this approach was
assessed. To this aim, an integrated approach was followed. The
ELFM used a wet technology, described in chapter 2.4.3.1, to max-
imize separation efficiency and provide contaminant-free materi-
als, depending on the intended use.
The use of wet technologies applied to waste separation has
been already documented in literature: Wanka et al. (2017) have
analyzed the wet treatment of excavated waste consisting mainly
of a separation of lightweight and inert fractions caused by a ver-
tical pulsating water stream in a jigger bed, followed by water
purification in a cyclone. The foreseen employement of the light-
69
weight fraction, containing plastic, has been the energy recovery,
while for inert materials recycling in the construction sector has
been advocated.
A different plant configuration has been described by
Kranzinger et al. (2018), where the wet treatment is performed
in an horizontal separator which uses centrifugal force to separate
a high polyolefin-concentration stream for thermochemical
conversion.
The Life Cycle Assessment (LCA) methodology was adopted to
analyse the environmental impacts and benefits deriving from
the ELFM applied to an industrial landfill located in southern Sar-
dinia, Italy, focusing on the valorisation of the plastic fraction
recovered.
The recovered plastic fraction was analyzed and a proper pro-
cessing strategy was designed, obtaining a secondary raw material
that competes with virgin LDPE in terms of properties.
Virgin, fossil-based LDPE was then used as a comparison basis
to evaluate the environmental benefit of ELFM derived secondary
raw material.
The valorization strategy implemented is based on additivation
and melt compounding and has been validated in terms of
mechanical properties of the recyclates. This study represents an
evolution of a previously published work (Cappucci et al., 2019),
in which the mechanical performance of the product had not been
taken into account. In this work, the mechanical performance of
the secondary material was almost completely equated to that of
a primary material. The LCA was then focused on the environmen-
tal impact of the production of a secondary plastic obtained with
ELFM rather than the impact associated with the state of the land-
fill, identifying the main contributions to the damage and benefits
associated with the operations of landfill mining. Possible environ-
mental benefits of the secondary raw material, compared with a
plastic product obtained from primary resources were addressed
and quantified.
2. Materials and methods
2.1. Materials
Waste plastic (WP) materials were provided by IREOS S.p.A.
(Genova, Italy). The plastic fraction was sorted during the mining
and reclamation activities carried out by IREOS on an unregulated
landfill site located in southern Sardinia (Italy).
The types of industrial waste found were mainly inerts (93.7% of
total treated waste), and high quantities of coal (4.6%) and alu-
minium (1.17%), resulting from an industrial decommissioning of
a company working on aluminium that occurred on the site. Other
types of waste were cathodes and anodes, plastics, electric cables,
iron, asbestos, tyres and wood. Each of them represented < 1% of
total treated waste. Quantities are listed in Table 1.
The multi-stage waste treatment process implemented is
schematized in Fig. 1.
Maleated linear low density polyethylene (MAPE), Compoline
CO/LL, with a grafted maleic anhydride content of 1.4 wt%, was
kindly supplied by Auser Polimeri S.r.l. (Lucca, Italy), and used as
an additive, to enhance the adhesion of the polyolefin fraction of
WP with polar organic and inorganic inclusions.
Low density polyethylene (LDPE), Hipten 21018, kindly sup-
plied by HIP Petrohemija AD (Pancevo, Serbia), was used as an
additive as well, to compare its effects with those of MAPE.
2.2. Techniques
Infrared spectra of randomly selected, as received WP frag-
ments were recorded on a Perkin Elmer Spectrum 100 FTIR spec-
70 G.M. Cappucci et al. / Waste Management 118 (2020) 68–78

Table 1 materials, by means of a Scanning electron (SEM) Quanta 200

Inventory of ELFM process. FEG microscope (FEI, Hillsboro, OR, USA) working in high vacuum
Input Value Unit mode with an acceleration voltage ranging from 10 to 30 kV and
Waste treatment 5.3E8 kg using a secondary electron detector. Before SEM observations,
Inputs from nature cryo-fractured surfaces were sputter coated with an Au/Pd alloy
Land occupation (industrial area) 3.6E4 m2a by means of an Emitech K575X sputtering device.
Land transformation (to industrial area) 1.2E4 m2 To obtain further information on WP composition, samples pre-
Land occupation (landfill) -4.7E5 m2a
Land transformation (from landfill) 1.6E4 m2
pared for morphological analysis were subjected to Energy disper-
Materials sive X-ray analysis (EDX), carried out by means of an Oxford Inca
Water 4.3E4 m3 Energy System 250 and an Inca-X-act LN2-free analytical silicon
Cement for plant base 2.9E6 kg drift detector (Abingdon, UK), in high vacuum mode at 30 kV accel-
Fuel oil for conditioning 3.3E4 kg
eration voltage.
MIBC 7.3E3 kg
Flocculant 1.5E4 kg
Fuel oil for machinery 3.8E5 kg 2.3. Valorization process
Cement for waste inertization 3.4E6 kg
Energy Materials received from the ELFM site were subjected to a
Electricity 4.9E6 kWh
grinding step in a rotary knife mill (Retsch SM100) with a 2 mm
Trasports
Road 1.5E10 kgkm bottom sieve, to homogenize the composition and granulometry
Ship 1.8E11 kgkm for subsequent processes.
Ground WP was then melt processed in an internal mixer
Output Value Unit
By-products (Brabender Plastograph EC, Brabender GmbH, Duisburg, Germany)
Iron 3.1E6 kg at 190 °C/60 rpm, pelletized and compression molded at 190 °C to
Aluminium 6.2E6 kg produce 1.5 mm thick sheets. This batch processing route was
Plastic (PE) 5.9E5 kg
selected to meet the needs of lab-scale operations, however for
Carbon 7.1E6 kg
Electric wires for copper recovery 9E3 kg LCA calculation the typical parameters of industrial-scale, continu-
Emissions to air ous extrusion were considered as described in the cap. 2.4.3.2.
Ammonia 1.1E-1 kg Based on previous studies (Avella et al., 2009; Avolio et al.,
Metals 4.2E-2 kg 2015) maleated polyethylene (MAPE) was tested as additive in
Hydrocarbons 1.8E-4 kg
the concentration range 2.5 – 5 wt%, selected on the basis of previ-
Asbestos fibers 1.5E-5 kg
Fluorides 3.3E-2 kg ous studies ((Avolio et al., 2019); (Lai et al., 2003)) and of the
Wastes amount of polar inclusions in WP (about 10 wt%, see Section 3.1.1).
Wood composting 6.45E4 kg To confirm the effect of reactive groups of MAPE vs. a possible
Tyres treatment 1E5 kg
action through dilution or molecular weight distribution changes,
Recycling of building materials 2.9E6 kg
Treatment of electronic components 4.4E6 kg
WP additivated with plain, virgin PE was also produced.
Landfilling of non-recoverable waste and covering soil 5.4E8 kg
Incineration of packaging plastics for energy recovery 8E3 kg 2.4. Life cycle assessment
Asbestos treatment 1.2E5 kg
Wastewater treatment 9.2E9 kg
2.4.1. Definition of objective and purpose
The objective of the study is the environmental impact assess-
ment through the LCA methodology according to UNI EN ISO
trometer (Waltham, MA, USA), equipped with an attenuated total 14040-14044 (UNI EN ISO, 2006a, 2006b) of the damage due to
reflectance accessory (ATR). All spectra were recorded in the the treatment of waste from an industrial landfill and the produc-
4000  400 cm 1 range with a resolution of 4 cm 1, averaing 16 tion of secondary plastic material, starting from the recovered WP
scans. whose overall properties were improved through the addition of
Solid state 13C MAS NMR spectra were collected on a Bruker chemicals and execution of additional manufacturing processes.
Avance II 400 spectrometer (Bruker Biospin, Billerica, MA, USA),
equipped with a 4 mm MAS probe. Ground WP samples were 2.4.2. System, functional unit and function of the system to be studied
packed into 4 mm zirconia rotors sealed with Kel-F caps and spun The function of the system is the production of secondary plas-
at 10 kHz. Cross-polarization (CP) spectra were recorded with a tic material, in particular PE granules, with primary product-like
relaxation delay of 5 s and a contact time of 2 ms, under high mechanical performance, obtained through the excavation and
power proton decoupling. Spectra were referenced to external treatment of the waste contained in the industrial landfill and sub-
adamantane, (CH2 signal at 38.48 ppm downfield of TMS, set at sequent processing of the recovered fraction.
0.0 ppm). The system studied is the industrial landfill mining operated by
Thermogravimetric analysis (TGA) of compression molded WP IREOS S.p.A. in Portovesme, part of the Municipality of Portoscuso
was carried out on a Perkin Elmer Pyris 1 TGA (Waltham, MA, (SU). The production of secondary plastic material is performed by
USA) using air as purge gas and a linear heating ramp from 40 °C a hypothetic company located in Naples, which receives the plastic
to 800 °C at 10 °C/min. by-product resulting from landfill mining operations.
Tensile tests were performed on dumb-bell specimens (6 mm2 The Functional Unit is 1 kg of finished secondary plastic
cross section, 1.5 mm thickness, 26 mm gauge length) obtained granulate.
from compression molded sheets of WP and WP-based materials
at 10 mm/min deformation speed, on a 5564 Instron testing 2.4.3. System boundaries
machine (ITW Inc. Glenview, IL, USA). Young’s modulus (E), peak The production of a secondary plastic material was taken into
stress (rmax) and elongation at break (eR) were calculated as aver- account, considering the ELFM operations to recover the plastic
age values over at least 6 tested samples. waste and the necessary mechanical-chemical treatments for its
Morphological analysis was carried out on cryogenically valorisation, starting from the excavation of waste from the landfill
fractured surfaces of compression molded WP and WP-based site, the treatment with specific machinery, the disposal of non-
 G.M. Cappucci et al. / Waste Management 118 (2020) 68–78 71

Excavation Emissions zone 1

Waste Covering soil Inertization

Bulky waste (tyres, coarse

iron, wood, cathodes and
Mechanical sorting Disposal/recycling
anodes, packaging platics,
electric wires, asbestos)
Dry treatment
Emissions zone 2
(grinding)

Primary sieving

Fraction > 150 mm Fraction < 150 mm

Magnetic separation Wet pre-treatment

(eddy current system) (grinding)
Fraction = 30 mm
Magnetic separation
Aluminium Bulky plastic (eddy current system)

Grinding
Non metals (inerts) Metals (aluminium, iron)

Vibrating wet sieving

Fraction 0-1 mm Fraction 1-30 mm

Hydrocycling Gravimetric separation

Fine fraction Ultrafine

fraction Water Plastic Coal Sink Middling

Conditioning
Disposal after inerting

Floatation Emissions zone 3

Water Coal Sand

Treatment Disposal

Sludge Purified water

Disposal after inerting

Fig. 1. Schematic representation of the landfill mining approach examined in this paper.

recoverable waste and the obtaining of by-products from the
remaining waste to be further valorized.
The production, maintenance and disposal of machinery and
other auxiliary materials were included in this study. Air and
indoor emissions as well as the production of solid and liquid
waste were considered and quantified. In addition, the following
assumptions were made:
 Transport of raw materials, plant, systems and machinery at an
average distance of 100 km from the producer to the user.
72 G.M. Cappucci et al. / Waste Management 118 (2020) 68–78
 Installation of HEPA filters (High Efficiency Particulate Air fil-
ters) with an efficiency of 99.97% during the production of sec-
ondary granulate.
 The use of personal protective equipment of the facial type with
an efficiency of 95% during the production of secondary granu-
late according to European standards (UNI EN, 2009).
2.4.3.1. Treatment of landfill waste. The ELFM process performed by
IREOS S.p.A. consisted of various treatment phases, starting with
the excavation of the landfill and characterized by a patented
wet-processing technology called ‘‘TWYM: Tomorrow’s World,
Yesterday’s Materials” (patent nr. 102,015,000,089,311 of italian
Ministry of Economic Development, Tealdo, 2018), that allowed
to recover high quality materials. In particular, the PE recovery effi-
ciency is estimated to be at least 80%.
The technology is a gravimetric technology that uses water as a
dense fluid, moving the material with air under pressure. The
water separates the different materials, but at the same time
washes the material itself, removing the contamination, which as
usual in a soil washing platform, concentrates in the final mud.
The treatment of the excavated waste was performed within an
on site installed modular plant, thus minimizing the transport of
materials. A flowchart of the process that includes the specific
treatment phases is reported below, highlighting for each of them
the waste flows and any direct emissions (Fig. 1).
There was an emission abatement system on dry activities con-
sisting of a cannon fog, which sprays water and wets the material
so as to limit the dispersion of dust in the environment generated
during the mining activity.
As shown in Fig. 1, excavation of landfilled waste preceded dry
and wet treatments. During this phase, emissions of metals
(arsenic, cadmium, nickel, lead, copper, zinc and aluminium), poly-
cyclic aromatic hydrocarbons, ammonia, aero-dispersed asbestos
fibres and fluorides occurred (zone 1) (CPG Lab Srl, 2017).
In the mechanical sorting, performed with tracked construction
machine equipped with bucket, process bulky waste such as tyres,
wood, coarse iron, asbestos, electrical cables, packaging plastics,
cathods and anods were removed from the remaining waste, that
will be subjected to the next treatment phases. In the area used
for unloading and screening materials the above mentioned pollu-
tants for zone 1 were measured (zone 2).
The gravimetric separation in water aimed to separate the tar-
get plastic from the remaining waste, on the basis of the difference
in density of the treated materials.
The process, in fact, was based on the operation of stratification
of materials that took place inside the machine: thanks to a move-
ment generated by the pressurized air, low-density materials strat-
ified on the surface of the fluidized bed, while high-density
materials stratified on the bottom. The machine has at the dis-
charge many output channels as the number of output fractions.
The output channels are located at different heights of the machine
depending on the waterline of each fraction.
The resulting target plastic matrix underwent further refining
within the gravimetric separation, which removed any further cel-
lulosic contaminants and earthy residues.
Any finer material was removed from water through a hydro-
cycling process, which allowed the separation of an ultra-fine frac-
tion from the remaining waste and then with a floatation (the most
significant emission source in zone 3) in order to have a subse-
quent separation between the float and the sands. A conditioning
step, in which additives such as diesel fuel and MIBC (methyl-
isobutyl-carbinol) were added as frother agents for the hydropho-
bisation of sand and coal, was a necessary preparation for the fol-
lowing flotation.
The water used in wet treatments and containing the contami-
nants washed away from the waste, was treated in a clarification
plant, with chemical-physical treatment and sludge filter-
pressing processes, and, subsequently, recirculated in the waste
treatment plant.
In addition to plastic, the by-products of the treatment activity
were a carbon fraction with a high calorific value for energy recov-
ery, and recyclable ferrous and non-ferrous metals. These fractions
were considered as by-products of the treatment process because,
thanks to any further enhancement processes, they still had a mar-
ket value and could provide secondary material or energy, as
opposed to waste that is mostly landfilled at the end of treatment.
The transport of by-products was considered, in particular the
ship transports of plastics and carbon fraction, respectively to
Naples, where experimental tests on materials have been carried
out, and to Lisbon, where energy recovery was performed, while
for metals a transport of 100 km was supposed.
The destination for waste generated at the end of treatment and
for non-recoverable materials varied according to the type of
waste.
Landfilling was foreseen for sludge generated by the filter-
pressing of the water treatment plant, the sand, the ultrafine frac-
tion, the mixed material consisting mainly of crushed stone, con-
crete and refractory materials with an irrelevant carbon content
(sink), the inerted covering soil and the mixed material with a
medium carbon content (middling), that was made inert with
cement addition and landfilled in the city of Nerva, Spain.
The ‘‘irrelevant” content of carbon in the sink means no more
than 150 ppm. The average carbon content is in the ‘‘medium” frac-
tion, and in this case the quantity is very high, almost 20% by mass.
Waste recovered with mechanical sorting such as tyres, cath-
odes and anodes, asbestos and wood, were subjected to specific
treatments, instead part of the packaging plastics were burnt for
energy recovery and the most contaminated packaging plastics
were landfilled.
The removal of asbestos from the landfill body was carried out
by qualified personnel, who encapsulated the asbestos slab first by
spraying a silicon oxide made primer and then by wrapping it in an
LLDPE sheet. Following the removal of the slab, it was supposed to
be thermally inert (Gualtieri, 2006).
2.4.3.2. Valorization of WP. The plastic fraction, recovered at the
end of the treatment (WP) and consisting of 90% PE (with the
remaining 10% represented by other materials, as detailed in Sec-
tion 3.1.1), was transported to the processing site.
The industrial scale valorization/processing procedure was
schematized as follows.
The first stage of processing consisted of a grinding phase that
reduces the size of the input fraction, in order to obtain a 1 cm size
intermediate product. A sieve separated the fraction sizing less
than 1 cm, estimated to be about 90%, which was directed with a
conveyor belt to the next stage of extrusion, from a sieving residue.
The sieving residue was made of a coarser fraction (sizing more
than 1 cm and supposed to be 70% of the sieving residue), which
was cycloned to separate it from a possible fine portion and, then,
grinded again.
5% by weight of MAPE (better performing composition, see
Table 3) was added to the WP, with the aim to control morphology
and improve the properties of the final product. The mixture of WP
and MAPE was processed at 180 °C and 80 bar in a single-screw
extruder equipped with a filter to remove solid impurities, granu-
lated and cooled with water in a closed circuit.
Each phase of processing of the recovered plastic was equipped
with dust emission suction systems, whose entity was evaluated
considering a percentage of the treated plastic.
 G.M. Cappucci et al. / Waste Management 118 (2020) 68–78 73

2.4.4. Data quality Table 2

Primary data about waste treatment were collected thanks to Inventory of the production of the secondary plastic granulate.

direct interviews with IREOS S.p.A., concerning the treatment Input Value Unit
phases, description of the machinery, energy and water consump- Materials
tion, emission concentrations and quantities of separated materials PE recovered with ELFM 1.06 kg
at the end of the treatment. All the chemical analysis have been MAPE 4.8E-2 kg
done by a chemical independent laboratory. Moreover, during all Energy
Electricity 0.46 kWh
the activities, there was the control of Local authority, because Trasports
the activity was located in a SIN (Sito di Interesse Nazionale - Road 120 kgkm
National Interest Site). The ARPAS (Agenzia Regionale per la Prote- Ship 540 kgkm
zione dell’Ambiente della Sardegna - Regional Agency of Environ- Output Value Unit
ment Protection of Sardinia) has checked itself all the samples Product
with independent chemicals analysis. PE granulate 1 kg
The production process of the secondary granulate was outlined Avoided product
Waste plastic recovered 7.4E-2 kg
through interviews with a company that processes plastic
Emissions to air
materials. Particulates 9.76E-6 kg
The adopted database was Ecoinvent v. 3.5 (Ecoinvent Center, NMVOC 5.4E-5 kg
2018). The damage assessment method was IMPACT 2002+ Particulates, indoor 1.58E-10 kg
(Jolliet et al., 2003) modified in agreement with Pini et al. (2014). Waste
Disposal of particulate matter retained by 3.2E-2 kg
The calculation code used was SimaPro 9 (PRé Consultants,
bag filters in landfills for hazardous waste
2019). Since the IMPACT 2002+ method did not take into account Waste plastic recycling 3E-3 kg
local and indoor emissions, in particular, in relation to particulate
matter emitted during grinding and inhaled by workers, character-
isation factors were calculated by adopting a preliminary method
(Ferrari et al., 2019), in order to assess the human health effects
After the preliminary grinding, 13C solid state NMR spectra were
of these emissions.
recorded on WP powder to further clarify its composition. As
The impact category Mesothelioma and the damage category
shown in Fig. 2, the main peaks of polyethylene were recognized,
Cancer due to asbestos fibres were taken into account to consider
with very low amount of polypropylene (<1 wt%, weak signals at
the human health impacts of asbestos fibre emissions (Cappucci
44 and 22 ppm partly covered by the broad PE peak), cellulose
et al., 2019).
( 1.5 wt%, signals at 74 and 65 ppm) and polystyrene (<1 wt%,
The model used for the Life Cycle Inventory (LCI) was attribu-
main signal at 130 ppm).
tional, partitioning, in order to manage the presence of by-
It is important to note that the thorough washing implemented
products resulting from waste treatment activity, according to
in the selection process led to WP with a much lower content of
the assessment requirements (Pini et al., 2018).
contaminants, both organic and inorganic, with respect to the
The allocation was based on the mass criterion, as it was consid-
‘‘raw” plastic stream analyzed in a previous paper (Avolio et al.,
ered the best principle to distribute the damage between different
2019). While polymeric and cellulosic contamination was quanti-
types of by-products. This criterion was recommended by UNI EN
fied by NMR, the amount of inorganics (essentially silicates due
ISO 14040 (UNI EN ISO, 2006a, 2006b) and, moreover, allows all
to soil and dust residues, as identified by EDX analysis in Sec-
by-products to be assigned the same value, since each of them
tion 3.1.2) was evaluated by weight loss curve (TGA analysis)
required further treatment to obtain secondary material.
recorded in oxidizing atmosphere. The residual weight at 800 °C,
after complete combustion of the organic fraction, was found to
2.4.5. Inventory be 6.5 wt%. The amount of polar contaminants plays an important
The most representative data used in the inventory of landfill role in the definition of final properties, as discussed in the follow-
waste treatment and granulate production are given in the follow- ing of this section.
ing tables (Table 1 and Table 2). Codes and compositions of the prepared materials are resumed
As a consequence of the recovery of recyclable materials and in Table 3.
the treatment of the remaining matrices, it was possible to appre-
ciate a volumetric reduction in waste equal to 37% of the initial vol-
3.1.2. Mechanical and morphological analyses
ume of the landfill and, therefore, a reduction in land occupation.
After melt processing and compression molding, all materials
Thus, the presence of a negative entry in the inventory for land
were characterized by means of tensile tests. The main mechanical
occupation and of the transformation from landfill (to which the
parameters are resumed in Table 3.
method gave negative value).
Neat WP shows a low elastic modulus and a moderate strength,
with values in the same range of the low density polyethylene
3. Results and discussion (Mantia et al., 2013; Sutivisedsak et al., 2012). The elongation at
break recorded on WP is surprisingly high, pointing out its high
3.1. Lab-scale recycling and testing of WP chemical purity; it is significantly lower than that of (L)LDPEs,
though. The addition of maleated polyethylene as additive induced
3.1.1. WP analysis and processing a strong increase in elongation, dependent on MAPE content,
The composition of the WP received was analyzed by means of reaching a value higher than 200% at the highest MAPE load. The
infrared spectroscopy carried out on several randomly selected effect of MAPE on the other parameters was much less significant,
plastic fragments (Fig. 2). All of the tested films were identified with a slight decrease of elastic modulus and an increase in
as polyethylene, with a surface contamination of soil residues strength.
and/or cellulosic material (revealed by the absorption peak at  In order to better clarify the role of polar groups of MAPE on the
500, 1000, 1600–1700, 3400 cm-1). ((Song et al., 2012); (Zhang final properties, neat LDPE was also used as additive. In fact, con-
et al., 2017); (Castaldo et al., 2019)) sidering that an overall decrease of molecular weight can be
74 G.M. Cappucci et al. / Waste Management 118 (2020) 68–78

Fig. 2. a) FTIR spectra recorded on different film fragments. Absorption peaks attributed to polyethylene and to contaminants are identified. b) Solid state 13C NMR spectrum
of ground WP compared to neat LDPE as a reference. In the magnified insert, the signals of main contaminants are identified (Cellulose is abbreviated as Cel). Spinning
sideband are marked by a dot.

Table 3
Codes, composition and mechanical parameters recorded on all tested samples: elastic modulus (E), peak stress (rmax), elongation at break (eR). Typical parameters of LDPE are
reported as a reference (from (Mark, 2007)).

Code Additive Pre-treatment E (MPa) rmax (MPa) eR (%)

Neat WP – – 165 ± 7 9.7 ± 0.1 70 ± 12
2.5 MAPE MAPE 2.5 wt% – 148 ± 6 10.0 ± 0.1 145 ± 32
5 MAPE MAPE 5 wt% – 143 ± 6 10.2 ± 0.4 229 ± 35
5 LDPE LDPE 5 wt% – 112 ± 6 8.9 ± 0.6 134 ± 91
LDPE (typical) – – 140–300 7–17 200–900

expected in WP, due to the uncontrolled storage conditions of the
landfill, the beneficial effects recorded as a result of the MAPE addi-
tion could in principle be also ascribed to an average molecular
weight increase. Testing LDPE as additive ruled out this hypothesis,
as it induced some increase in elongation at break (with a large
variability among the specimens, as indicated by the high experi-
mental error), but also caused a strong drop in elastic modulus
and strength. MAPE is widely recognized for its ability to enhance
adhesion of polyethylene with polar organic or inorganic fillers,
thus increasing the mechanical performances of composites
((Nwabunma, 2007); (Avella et al., 2009); (Mengual et al., 2017)).
LDPE, on the other hand, is not expected to modify adhesion: the
different tensile behavior of MAPE and LDPE containing samples
gives then a clear indication that the critical factor triggering the
premature break of WP is the presence of polar inclusion/contam-
inants, rather than molecular weight degradation induced by
aging. This lead to the conclusion that even if a thorough washing
step greatly reduced contaminants, in comparison to the raw
material examined previously by Avolio et al. (2019), contamina-
tion level still controls the final properties of recycled WP, and
the additivation with MAPE is able to greatly counteract its effects.
Scanning electron microscopy and EDX analysis were per-
formed on cryogenic fracture surfaces of selected WP samples (mi-
crographs are reported in Figure S1). Some high contrast particles
of micrometric size, probably soil particles, can be observed on
the examined surfaces, while, interestingly, larger (tens to hun-
dreds of mm) inclusions are absent in both samples. EDX analysis
allowed to define the nature of these micrometric inclusion,
revealing that the main inorganic elements present in WP samples
are, silicon, aluminum, calcium, iron, magnesium, sodium and
chlorine. This composition is compatible with soil residues and
inorganic salts (sodium chloride is an expected contaminant as
the reclaimed landfill is close to the sea). No heavy metal content
was evidenced in WP, within the detection limit of EDX.
Summarizing, the ELFM recovered plastics is mainly composed
of PE, with a relatively low amount ( 10 wt%) of other organic and
inorganic substances. As a consequence of the high purity of WP,
the simple additivation strategy proposed (based on MAPE) was
very effective, enabling the realization of a recycled material with
optimized properties.
3.2. Damage analysis
The environmental analysis of the damage caused by the extrac-
tion and treatment of 1.06 kg of PE, i.e. the amount of resource
required for the production of 1 kg of secondary PE, is given below.
The end-point damage is 1.83E-5Pt2, of which 54.6% is due to the
treatment of non-recoverable waste, 27.4% is due to the transport
of non-recoverable waste to a specific treatment/disposal, and more
than 8% is due to the use of electricity. The environmental advantage
deriving from the land release thanks to the waste volumetric reduc-
tion is equal to 0.36%. The results of the mid-point analysis, in
which the results are expressed in impact categories and quantified
in kg of reference substance for each category, are shown in Table S1.
Fig. 3 shows that the most significant contribution to the total
damage is provided by the category Global warming (29.45%),
due to the emission of carbon dioxide of fossil origin (79%), emitted
mainly in the processes of waste treatment and, in particular, the
treatment of cathodes and anodes.
The category Respiratory inorganics (29.2% of total damage) is
the second largest contributor to total damage, mainly due to the
emission of nitrogen oxides (36%) in waste transport processes,
in particular of middling and sludge to Spain by ship.
The category Non-renewable energy accounts for 20.4% of total
damage, mainly from the use of crude oil (69%), especially in
2
Pt is the abbreviation of ‘‘points”.
 G.M. Cappucci et al. / Waste Management 118 (2020) 68–78
6.00E-06
5.00E-06
4.00E-06
3.00E-06
Pt
2.00E-06
1.00E-06
0.00E+00
-1.00E-06
Excavaon Water
Electricity Waste treatments
Fig. 3. Damage assessment for impact category weighing of the ELFM process.
disposal of materials that could not be recovered, in particular
sand.
The category Non-carcinogens accounts for 10% of total damage,
mainly due to the emission into water of antimony (68.5%), emit-
ted mainly in the end-of-life treatment process of anodes and cath-
odes, supposed to be a shredding of used electronic products. This
treatment was schematized with an Ecoinvent database process,
that takes into account long-term emissions from landfilling of
residues of incineration (activity of waste disposal of residue from
shredder fraction from manual dismantling).
The Terrestrial ecotoxicity category contributes 4.7% to the total
damage, mainly due to the emission of zinc into the soil (35%),
especially in the treatment of non-exhaust emissions produced
by abrasion from tyres of vehicle, in particular, caused by sand
transport by road to the new landfill site.
The category Carcinogens accounts for 2.36% of total damage,
mainly from the emission of aluminium into the air (27.9%), in par-
ticular in the end-of-life treatment process of anodes and cathodes.
In particular these emissions occurred during the blasting process
for zinc extraction. The shredding process of Ecoinvent database
consideres zinc as an alloying metal for the remelting of alu-
minium scraps (one of the processes of the dataset of shredding
of used electronic products).
The other categories contribute less than 2%.
The end-point analysis of secondary PE production (Table 4), in
which the results are normalised and expressed in Point, which
represents the average damage in the specific category caused by
a person in one year in Europe, shows that the total damage for
the production of 1 kg of granulate is equal to 1.98E-4 Pt, due to
extrusion and granulation with 38.3%, followed by the grinding
process with 31.6%, that includes the plastic extracted from the
landfill, the MAPE addition with 21.5% and, finally, packaging with
8.5%.
In particular, the damage categories that contribute most to the
total damage are Resources (39.1%), mainly due to Oil, crude
(32.2%), used mainly for the production of MAPE. Human health
75
Dry treatments Wet treatments
Transports Others
(32.88% of total damage) is mainly affected by the emission into
the air of particulate matter < 2.5 lm (28%) which is emitted for
about 38% for energy used in extrusion. The contribution to the
total damage of Climate change (22.98%) is mainly due to carbon
dioxide, fossil (93.3%), emitted mainly in the extrusion phase
and, in particular, for energy used in extrusion.
The damage in Ecosystem Quality (5.06% of the total damage) is
mainly due to the intensive occupation of forest for chips produc-
tion (15.6%), due to energy used in extrusion.
Human health on an indoor scale (6.9E-5%) is mainly affected by
particulate matter >10 lm (32.4%), emitted almost entirely directly
during grinding.
The category Cancer due to asbestos fibers (7.9E-8% of total
damage), whose damage is due to the treatment of waste from
landfill and, in particular, to wet treatment, contributes only to
the damage of the grinding phase. Finally, Human health on a local
scale (1.96E-10% of total damage) is due for 59.3% to particulate
matter >10 lm, emitted in the regeneration process of spent active
carbon resulting from the filtering in extrusion process.
The damage related to the extraction and treatment of PE con-
stitutes the second contribution to total damage (29.3%) of the
grinding phase for the production of secondary granulate, preceded
by used energy (32.9%) and followed by transports (27.9%) (Fig. S2).
PE recovered with ELFM is also an avoided product, as, thanks to
screening, it is possible to recover part of the waste resulting from
grinding and put it back into the production process.
In order to assess the environmental sustainability of the gran-
ulate produced from PE recovered from landfill compared to the
granulate produced from virgin LDPE and secondary PE obtained
from conventional recycling, the following comparison between
the two scenarios just mentioned is reported below (Fig. 4). Since
the database does not include an LDPE recycling process, it
assumes HDPE recycling as a proxy.
The process that has the greatest impact is the production of
virgin LDPE according to the database process (Ecoinvent Centre,
2018), in particular it is more than 4.46 times greater (8.8E-4 Pt)
76 G.M. Cappucci et al. / Waste Management 118 (2020) 68–78

Table 4
Single score analysis of the secondary granulate production.

Damage category Unit Total Grinding MAPE Extrusion Packaging

Resources Pt 7.75E-05 1.80E-05 2.44E-05 2.65E-05 8.59E-06
Human health Pt 6.52E-05 2.45E-05 8.96E-06 2.74E-05 4.36E-06
Climate change Pt 4.56E-05 1.59E-05 8.87E-06 1.72E-05 3.61E-06
Ecosystem quality Pt 1.00E-05 4.26E-06 4.34E-07 4.96E-06 3.82E-07
Human health, indoor Pt 1.37E-10 1.37E-10 0 4.05E-19 0
Cancer due to asbestos fibers Pt 1.57E-13 1.55E-13 0 1.88E-15 0
Human health, local Pt 3.88E-16 0 0 3.88E-16 0

1.00E-03
9.00E-04
8.00E-04
7.00E-04
6.00E-04
Pt

5.00E-04
4.00E-04
3.00E-04
2.00E-04
1.00E-04
0.00E+00
Secondary HDPE granulate (R) Secondary PE granulate (ELFM) Primary LDPE granulate

Human health Ecosystem quality Climate change

Resources Human health, indoor Human health, local
Cancer due to asbestos fibers

Fig. 4. Comparison of damage assessment for single score between secondary HDPE granulate production from conventional recycling (R), secondary granulate production
from ELFM (ELFM) and primary LDPE granulate production.

than the production of granulate from recovered WP. In particular,
the increases for the following categories of damage can be noted.
For Resources, the damage of the virgin production case is 6.6
times greater (5.1E-4 Pt) than that of the recovered WP (7.75E-5
Pt), in particular for crude oil consumption (2.5E-4 Pt against
2.6E-5 Pt in the recovery scenario) which in the database process
represents the main resource for the production of virgin LDPE
(in fact, to obtain 1 kg of virgin LDPE 0.84 kg of crude oil is
required). For the production of secondary PE, crude oil is used
mainly for the production of MAPE.
For Human health the damage of virgin granules is 2.75 times
greater (1.79E-4 Pt) than in the case of landfill recovery (6.5E-5
Pt), in particular for the damage due to the emission of aromatic
hydrocarbons (5E-5 Pt) which is an order of magnitude greater
than the WP recovered from landfill (3E-6 Pt), in particular because
of the direct emissions present in the database process.
For Climate change the damage of virgin granulate is more than
4 times greater (1.9E-4 Pt) than in the case of recovery (4.56E-5 Pt),
in particular by an order of magnitude per carbon dioxide, fossil
(1.7E-4 Pt) than in the case of recovery (4.2E-5 Pt), mainly due to
direct emissions present in the database process.
Ecosystem quality is 4 times higher in the case of WP recovered
from landfill (1E-5 Pt) than in virgin production (2.5E-6 Pt), espe-
cially for the intensive occupation of forest for chips production,
due to energy used in extrusion.
For the categories Human health on an indoor scale, Human
health on a local scale and Asbestos fibre cancers the damage is
considered only for recovered WP.
The secondary PE obtained from ELFM globally has a higher
impact compared to the traditional recycling process of 20.7%, in
particular the category with the highest increase is Resources
(+42%) for the use of crude oil in the production of MAPE. Climate
change is increased of 25%, in particular for the emission of fossil
methane and Human health is increased of 16.6%, mainly for the
emission of aromatic hydrocarbons, both emitted in the production
of MAPE. There is a trend inversion for Ecosystem quality, that is
reduced in the case of secondary PE from ELFM of about 136%: Alu-
minium emitted is soil results higher in the case of the traditional
recycling, in particular for an informal or uncontrolled burning of
waste that could be produced during recycling. An important point
about the concentional recycling database process is that machin-
ery is excluded, unlike the secondary PE from ELFM, where all the
infrastructures are considered.
4. Conclusions
The feasibility and environmental sustainability of the recovery
of a plastic waste fraction through ELFM and its valorization
through a proper processing were demonstrated by an integrated
experimental and LCA approach.
A treatment based on a simple additivation and melt com-
pounding was set up allowing the valorization of the ELFM recov-
ered plastics. The secondary raw material produced showed
mechanical properties comparable to that of a primary material.
The importance of contaminants such as other plastics, cellulose
 G.M. Cappucci et al. / Waste Management 118 (2020) 68–78
and earthy residues, as well as the role of adhesion-promoter addi-
tives on properties was pointed out, highlighting the importance of
washing and additive selection for the recycling of WP. Though a
detailed analysis of potentially harmful contaminants was not car-
ried out, no heavy metals were evidenced in WP, within the detec-
tion limit of EDX.
LCA highlighted that the recovery scenario is environmentally
preferable from two points of view: one related to the use of
resources, the other to the presence of emissions. In fact, the
strength of the production of the secondary resource lies in the
avoidance of the extraction of non-renewable resource (crude oil)
and emissions from the crude oil refining process.
If the production process of secondary granules is specifically
analysed, one of the main relevant step is the grinding of the
incoming waste, in which the ELFM process for the recovery of
the plastic fraction covers represents the 29.3% of the grinding
damage. The indoor human health category, which quantifies the
damage caused by inhaled emissions from workers, was included
in this study and its contribution to the total damage is limited,
equal to 6.9E-5%, thanks to the presence of extraction systems
placed on each machine and the use of personal protective
equipment.
The main contribution to total damage is provided by extrusion,
due to the high energy consumption of the machine, followed by
grinding phase and MAPE addition, for the production of MAPE
itself.
The main contribution to the ELFM is attributable to the dis-
posal of non-recoverable waste, in particular the treatment of cath-
odes and anodes and the landfilling of sand, followed by transports
of non-recoverable waste, in particular for middling and sludges by
ship - due to the long distance to the disposal plant- and for sand,
due to its great amount.
The environmental benefit of avoiding land occupation by
reducing the volume of remaining waste was included in the anal-
ysis and was found to be 0.36% of the damage from ELFM
operations.
Damage mitigation options for the ELFM process mainly con-
cern the treatment of non-recoverable waste, especially sand. If
subjected to a more thorough washing to reduce contaminants,
sand could be used to make road subfloors or, under appropriate
verification of suitability, in the construction sector, thus becoming
a by-product of the treatment process. In addition, its transport
would also be significantly decriminalised.
Funding
This research was partly funded by the Italian Ministry of
Economic Development (MISE) in the frame of the Horizon
2020-PON-MISE 2014/2020 project ‘‘Ideazione e sviluppo di un
innovativo Sistema multifunzionale polivalente finalizzato alla
valorizzazione di materiali plastici di scarto, recuperati principal-
mente da depositi interrati e/o discariche, ai fini di un loro riuti-
lizzo e/o impiego in specifiche filiere”, DD 22/12/2016, pos. 219.
Declaration of Competing Interest
Patent of one of the authors (Gianluigi Tealdo). Tealdo, G., 2018.
Procedimento per la bonifica di discariche. patent nr.
102015000089311 of italian Ministry of Economic Development.
Appendix A. Supplementary data
Supplementary data to this article can be found online at
https://doi.org/10.1016/j.wasman.2020.07.048.
77
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