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Resources, Conservation & Recycling 155 (2020) 104646

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Resources, Conservation & Recycling


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

Design from recycling: A complex mixed plastic waste case study T


a, b a a c b
Kim Ragaert *, Sophie Huysveld , Gianni Vyncke , Sara Hubo , Lore Veelaert , Jo Dewulf ,
Els Du Boisc
a
Department of Materials, Textiles and Chemical Engineering, Research Group CPMT, Ghent University, Technologiepark 130, Ghent, Belgium
b
Department of Green Chemistry and Technology, Research Group STEN, Ghent University, Coupure Links 653, Ghent, Belgium
c
Product Development, Faculty of Design Sciences, University of Antwerp, Antwerp, Belgium

A R T I C LE I N FO A B S T R A C T

Keywords: With today’s continued drive to increase recycling rates of plastics, the low-hanging fruit of clean mono-streams
Mixed plastic waste of plastic waste has long since been picked. If Europe’s ambitious recycling targets are to be met, plastics waste
Design from recycling streams that have until now been labeled ‘problematic’ and have consistently been sent to incineration, must be
Mechanical recycling considered as well. One such stream is the sink fraction obtained from float-sink sorting of mixed post-consumer
Product development
packaging waste. It is a very complex stream in terms of composition. Moreover, it contains a sizeable amount of
PVC, which is considered detrimental to further mechanical recycling of any mixed plastic waste. Within the
current research, the sink fraction was extensively analyzed for composition and mechanical properties, as well
as treated for removal of PVC and non-ferrous metals. Subsequently, the Design from Recycling strategy was
applied to successfully develop a new product with this material, called the Greentile. The Greentile was ef-
fectively manufactured and found to be a useful construction element for slanted green roofs.

1. Introduction new plastics packaging by 2030. Additionally, a recent amendment to


the Packaging and Packaging Waste directive (European Commision,
Plastics have been identified as one of the most promising materials 2018) has a heavy impact on how ‘recycling rates’ are allowed to be
to reduce the carbon footprint in Europe, alongside steel, aluminum and counted. Whereas previously, governments and EPR organization could
cement (Material Economics, 2018). Mechanical recycling of plastic count all the plastics that had been collected for recycling (baled after
waste is estimated to produce about 1.4 t CO2/t plastics, which is less sorting, so-called ‘exit sorting plant’), the amendment shifts this count
than 30 % of the CO2 emissions associated with making new plastics to those tonnages effectively going into a recycling operation, which
(5.1 tCO2/t plastics) (Material Economics, 2018). Yet still, only about will be considerably less as contaminations like labels and organic
30 % of all EU plastics are collected for recycling (Plastics Europe, debris are still to be removed. As such, there is still much gain to be had
2018) and of these, it is estimated that only 10 % is effectively recycled from increasing both quantities and qualities of recycled plastics. If
into new products. Europe’s ambitious recycling targets are to be met, we can no longer
At the same time, Europe is currently taking a political and legis- afford to only consider the very best of waste plastics recovered for
lative lead in circularity for plastics. In 2015 the European Commission recycling, but we must also consider more complex and challenging
introduced the Circular Economy Package (European Commission, plastic waste streams. One of these is the sink fraction from post-con-
2016), which included measures that will stimulate Europe’s transition sumer mixed plastic waste, which is a complex blend of PET, PS, filled
towards a circular economy, with plastics being one of the key ele- PP, PVC and a variety of minor components. The industrial sorting
ments. This has since been crystallized into the Strategy for Plastics in a process to obtain this fraction has been previously described (Ragaert
Circular Economy (European Comission, 2018). Strategy targets include et al., 2017). In brief, the fraction is the undesired part from the flo-
55 % recycling of all plastics packaging by 2025 and recyclability of all tation of post-consumer mixed plastic waste, in which the unfilled

Abbreviations: ABS, poly(acrylonitrile-butadiene-styrene); EoL, End of Life; EPR, extended producer responsibility; FEM, finite element method; FTIR, Fourier
Transformed Infra-Red; GMA, glycidyl methacrylate; LCA, life cycle analysis; MDD, material driven design; MPO, mixed polyolefines; MA, maleic anhydride; NIR,
near infrared; PA, poly(amide); PBT, poly(butylene terephthalate); PC, poly(carbonate); PE, poly(ethylene); PET, poly(ethylene terephthalate); PLA, poly(lactic acid);
PMMA, poly(methyl methacrylate); POE, polyolefin elastomer; PP, poly(propylene); PS, poly(styrene); PVC, poly(vinyl chloride); SAN, poly(styrene-co-acrylonitrile);
SEBS, poly(styrene-co(ethylene-butylene-co-styrene)

Corresponding author.
E-mail address: kim.ragaert@ugent.be (K. Ragaert).

https://doi.org/10.1016/j.resconrec.2019.104646
Received 30 March 2019; Received in revised form 27 November 2019; Accepted 11 December 2019
Available online 23 December 2019
0921-3449/ © 2019 Elsevier B.V. All rights reserved.
K. Ragaert, et al. Resources, Conservation & Recycling 155 (2020) 104646

polyolefines (PP and PE) are extracted as so-called MPO. MPO is typi- efficient material use (EU, 2009). In Design from Recycling, however,
cally recycled into outdoor furniture, enclosures, livestock stable panels the secondary raw material is the starting point of a new product de-
or boards for terraces (Huysman et al., 2017). The sink fraction re- velopment. Key aspects of the strategy include a thorough character-
presents around 20 wt% of the total incoming mixed plastics and is ization of the recycled polymer, adapted product (and mould) design to
currently sent to incineration (Huysveld et al., 2019). Two components the recycled polymer’s properties and identifying acceptable (cost-ef-
of this sink fraction are – regardless of extrudate quality – a compli- fective) strategies for the upgrading of the material quality (to product
cation for further processing, being a contamination of non-ferrous requirements) where necessary. Roughly, two approaches can be con-
metals (mostly Al) and a significant amount of PVC in the polymer mix. sidered within Design from Recycling, namely: (i) the drop-in approach:
Aluminum would cause blockages on the extrusion equipment but can required material specifications are a given and the recycled material
be removed fairly straightforward via Eddy current. The PVC compo- must be upcycled up to specification, so that it can substitute virgin
nent is a different story altogether. Complete removal via known se- polymers and (ii) the material driven design (MDD) method (Karana
paration techniques (like NIR) is very challenging, as the polymer mix is et al., 2015): the properties of the recycled material are used as a
already flaked at this point (required for the earlier sink-float). Yet, the starting point for the development of a wholly new product.
PVC removal is an absolute condition for further processing via me- Previously, this strategy has already been successfully implemented
chanical recycling. PVC is known to have poor thermal stability, de- to realize a high-quality consumer product made from the manu-
grading severely in the temperature range of 250−320 °C (Lopez- facturer’s own production waste, following the drop-in approach
Urionabarrenechea et al., 2012). During degradation, HCl is released, (Ragaert et al., 2018).
which is both toxic and highly corrosive to the equipment. In the It is the goal of the current research to apply the MDD method
converting of virgin PVC, this is not an issue as the PVC is processed at Design from Recycling to develop a product, suitable for manufacture
relatively low temperatures (well below 200 °C) (Osswald et al., 2006), with the challenging sink fraction but different from typical ‘bulk’ so-
with the addition of stabilizers and in corrosion-resistant equipment. lutions like outdoor furniture. To this end, the sink fraction was treated
However, the sink fraction under investigation holds a majority of PET, to remove non-ferrous metals and PVC and extensively characterized in
meaning that it will have to be processed at temperatures over 250 °C terms of composition as well as mechanical properties. A new product
for proper melting of the PET, which is quite an overheating for the PVC was not only developed, but an injection mould was likewise designed
component (Ragaert et al., 2017). As such, the degradation of PVC and manufactured. Finally, a test series of the new product ‘Greentile’
would be accelerated, leading to even HCl development. The gas will was produced and evaluated. LCA studies for this new product have
not only have corrosive effects on equipment and lead to a general been considered a separate study (Huysveld et al., 2019) and will be
quality reduction of the extruded polymer, it is also a known catalyst part of the discussion rather than the focus of this manuscript.
for the degradation of PET (Brebu et al., 2004), the majority polymer in
this very blend. Additionally, other polymers like ABS – which is a small 2. Materials & methods
contamination in this mix – have been found to in turn accelerate the
degradation of the PVC by reducing the dehydrochlorination tempera- 2.1. Materials
ture (Liu et al., 2017). As such, a complex degradation interaction
would occur if the sink fraction were to be processed as such, with The used polymer waste stream is the sink fraction of a post-con-
ruined equipment and useless extrudate as a result. sumer plastic waste from the Netherlands, that has been put through
In the current research, the sink fraction can be abstracted to be a the sorting process (Ragaert et al., 2017) at the plant of a typical re-
heavily contaminated PET stream. Specifically for the recycling of PET, cycler (Eco-Oh!, BE). These are dominantly rigid plastics, foils tend to
HCl has been previously identified as one of the most problematic remain with the float fraction, due to their large surface area. It was
contaminants for recycling (Paci and La Mantia, 1998). Threshold va- delivered as washed and dried flakes sized 0−15 mm. Only flakes
lues for PVC in recycled PET have been described as low as 100 ppm larger than 4 mm were considered.
(Paci and La Mantia, 1999) or even 50 ppm (Awaja and Pavel, 2005). As a compatibilizer, SEBS-g-MA was used (Kraton FG1901) in a 2 wt
Even if the PVC were to be removed from the sink fraction, a complex % dosage. It is a linear triblock copolymer with a styrene content of 30
blend of different polymer types still remains. As polymers are essen- % and grafted with 1.4–2 wt% MA.
tially immiscible, the resulting extrudate is expected to exhibit poor
mechanical properties such as brittleness (Ragaert et al., 2018). A 2.2. Pretreatment
common approach to mitigate the immiscibility in recycled polymer
blends is the addition of compatibilizers. Typically, these additives are The as-delivered sink fraction was subjected to the following se-
comprised of a relatively non-polar backbone for dispersive interactions paration treatments:
with non-polar components (like PP) with grafted functional groups for
bonding or interactivity with polar components (like PET). They are • For the removal of non-ferrous metals: three successive passages on
intended to reduce interfacial tension and as such improve dispersive an Eddy current separator (CTP, BE) using a polar wheel (50 Hz,
mixing of the different components in the blend. Typical examples of 3000 rpm), a conveyor belt (20 Hz, 0.46 m/s) and a separation
compatibilizers include SEBS-g-MA (Dobrovszky and Ronkay, 2016; splitter at 42 °C, to remove the non-ferrous metal particles. The
Pracella et al., 2002; van Bruggen et al., 2016), SEBS-g-GMA (Pracella setup can process 83 kg/h and yielded 1.1 wt% of mainly aluminum
et al., 2002; van Bruggen et al., 2016), PP-g-MA (Champagne et al., particles from the sink fraction;
1999; van Bruggen et al., 2016; Wang et al., 2011, 2018) and POE-g-MA • For the removal of PVC: Autosort Flake system (Tomra, DE), using a
(Kuzmanović et al., 2018; Mi et al., 2019). These are relatively ex- 1200 mm vibrating chute combined with an ejection module with
pensive additives, however, with prices ranging from three- to seven- several valves. The ultra-high resolution NIR detection system in the
fold those of virgin polymers. It is therefore only economical to use electronic evaluation system directs the rejection and acceptance of
them in relatively small amounts (2−5 wt%), for fear of increasing the passing material particles using 4 bar compressed air at a 0.6 T/h/
price of the recyclate above that of virgin polymers (Ragaert et al., 1.2 m rate, which yielded 20.6 wt% assumed-PVC in the reject
2017). section.
Design from Recycling is a product development strategy (Veelaert
et al., 2017b, 2017a), strongly complimentary to the better-known 2.3. Compositional analysis
Design for Recycling, which focuses on product recyclability at EoL by
promoting easy separation of different materials and an all-round Identification of polymer composition in the as-delivered and

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K. Ragaert, et al. Resources, Conservation & Recycling 155 (2020) 104646

Table 1
Load cases FEM analysis on Greentile.
Load Case Description Simulated load

1 Walking during installation F = 1200N


2 Saturated substrate, vegetation and walking p = 120 kg/m², F = 1200N
3 Saturated substrate, vegetation and snow and wind p = 120 + 275 kg/m²
4 Saturated substrate, vegetation and snow and wind and walking (= case 3 + walking) p = 120 + 275 kg/m², F = 1200N

pretreated mix was done by a combination of FTIR and NIR. FTIR material assignment, a custom material was created in the database
spectra of material flakes were obtained on the Tensor 27 FTIR device with the experimentally-determined properties of the PVC-free sink
from Brüker, equipped with an ATR crystal, using Opus 6.5 software. fraction. Different load cases were simulated, including the weight of
Data were derived based on 16 scans, resolution 4 cm−1; in the range of the saturated (by water) substrate and vegetation, the possibility of a
4000 cm−1 - 600 cm−1, using a KBr beamslitter, comparing spectra person walking on the green roof (during installation or maintenance)
with the software polymer database. and the effects of snow and wind. For the load of walking on the roof a
All samples were selected using the manual increment sample di- reference was set of a person of 120 kg (includes tools and safety gear)
vision technique according to standard CEN/TS 16,011: 2013. 500 standing on a surface area of 10 × 10 cm². For the load of the saturated
sampled particles were tested for each mix (before and after sorting). substrate (thickness 8 cm) and vegetation the load was fixed according
The composition of the reject (positively identified as PVC) from NIR to data provided by the supplier of both products. This was converted to
sorting was tested on 100 particles, to evaluate the number of false a pressure of 120 kg/m². Wind and snow loads were fixed at 275 kg/m²
positives in the sorting. Compositional data is represented in wt%, according to relevant standards (NEN, 1991a, 1991b). The settings for
which is determined by recalculated number of particles via the re- the different load cases are summarized in Table 1.
spective polymer density. All simulations were performed under three possible inclination
As a final and more elaborate control, NIR spectra of every particle angles for the slanted roof: 15° (minimum inclination), 45° (frequently
in 990 g of the accept-fraction of the pretreatment were obtained by a used inclination) and 55° (maximum inclination for Greentile system).
stationary unit, sIRo by IoSys (University of Waegeningen, NL). There are three supports assigned to the simulated product, the first and
second being the contact area of the Greentile with the wooden support
battens, respectively in Y and Z direction and the third being the con-
2.4. Mechanical and physical properties
tact area of the overlap between two tiles.
Mechanical properties and density were determined on injection
moulded testbars. 2.6. Injection moulding of Greentile parts
Injection moulding of testbars was performed on an ENGEL 80 T
machine with 800 kN clamping force and a 35 mm diameter screw with The Greentile mould was designed in-house and manufactured in
a nozzle temperature of 250−260 °C, an injection speed of 80 mm/s, mould steel 2311 on a 1:4 scale, in order to obtain a proof-of-concept.
injection pressure of 815 bar, 10 s of holding pressure of 680 bar and 30 The scaling to smaller size was required to reduce costs and for the
s of cooling time in a 30 °C test-specimen mould. The material was dried mould to be useable on in-house labscale machinery. Greentile parts
in a hot-air dryer for 2.5 h on 150 °C prior to processing. The test were manufactured on an injection machine (Engel 80 T) with a 35 mm
specimen were dogbone shaped, following ASTM D638-14, with a diameter screw, combining the technique of intrusion with injection
rectangular section of 4 × 6 × 35 mm³ for tensile testing and rec- moulding in order to augment the maximal volume capacity of this
tangular bars (13 × 3 × 128 mm³) for impact testing. All samples were small lab machine. The material was dried in a hot-air dryer for 2.5 h at
conditioned at 23 ± 1 °C and 50 ± 10 % relative humidity for 48 h 150 °C prior to processing.
prior to mechanical testing. 8 s of intrusion at 320 rpm was followed by injection moulding in a
Following ISO 527-1:2012, tensile data were obtained using an heated mould cavity, with two temperature profiles. Set injection
Instron 5565 tensile apparatus with Bluehill 2.0 software, equipped temperatures were either 260 °C (with mould temperature 40 °C) or 280
with a 5 kN static load cell, manual clamping grips (70 mm distance) °C (with mould temperature 60 °C), with the temperature profile
and an extensometer type Instron 2620-602 with gauge length of 12.5 ramping up to this maximum in four steps of 10 °C. Dosing speed was
mm. Extensometer removal occurred at 2.2 % strain, testing speed was 320 rpm, injection speed was 50 mm/s, using a maximum injection
set at 2 mm/min for initial slope and raised to 20 mm/min after re- pressure of 1300 bar. The holding pressure for 3 s was 200 bar, the
moval of extensometer. The modulus was determined as a segment cooling time 20 s.
modulus in the 0.05 to 0.25 % strain range, the yield stress was de-
termined using the 0.2 % offset method.
3. Results and discussion
Impact strength was determined on a Tinius Olsen apparatus model
503 with a pendulum of 2 J (impact speed 2.91 m/s), according to ISO
3.1. Composition of the sink fraction
179-1:2000, on 2 mm type A- edgewise.notched specimen.
Density measurements were performed according to the ISO 1183:
The polymer particle distribution of the as-delivered sink fraction is
2011 immersion method.
shown in Fig. 1 (left).
All measurements were done on a minimum of seven samples and
The main polymers in the as-delivered sink fraction are PET and PP
are reported as mean +/- standard deviation. In the SPSS 25 software,
(filled – most likely talcum – so that density > 1). The remaining
significant differences (p < 0.05) are determined by an independent
fraction (‘other’) is identified as containing the polymers PMMA, PA,
student t-test using the 95 % confidence interval for the mean.
ABS, SAN, PC, PBT and PLA. PET clearly dominates the mix, with filled
PP as a second-largest fraction. This is coherent with expectations based
2.5. Product CAD design and FEM analysis on composition of consumer packaging other than unfilled PE and PP
(which goes to the float fraction). PET (other than bottles) is ubiquitous
Product 3D CAD design and FEM analysis of the designed product in tubs and trays, while filled PP (mostly black) is typical for thermo-
(Greentile) were performed in the software package Siemens NX.11. For formed meal trays and the PS is typical for yoghurt pots (Brouwer et al.,

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K. Ragaert, et al. Resources, Conservation & Recycling 155 (2020) 104646

Fig. 1. Polymer mass composition (wt%) of original sink fraction (left); sorting ratio of autosort low throughput sorting system (middle); polymer mass composition
of sorted sink fraction (right).

2018). The large amounts of PVC are somewhat unexpected, as not higher than the previously recorded limit of 1 ppm, it was considered
many packaging products are still made of PVC. The PVC presence is acceptable for a trial of further processing into a product for the fol-
attributed to push-through strips (medication), non-food packaging lowing reasons: (i) the very low thresholds of 50−100 ppm are set for
from import products and mis-sorting (by the consumer). The assorted pure PET, while this blend contains a significant amount of (much more
polymers in the ‘other’ fraction is likewise attributed to mis-sorting or inert) PP and (ii) it was not expected to be possible to further decon-
to less-frequently used packaging (PLA for fruits, PA for frozen goods). taminate the PVC content from the flaked mix at the time.
It must be noted that the ‘PET’ denominator at this stage also contains However, should the use of the sink fraction be established on an
all PET-based multilayers. With PET making up over 70 wt% of the mix, industrial level, it would be recommended to further reduce PVC con-
the sink fraction can be considered as a heavily-contaminated PET tent. An effective way to achieve this would be not to sort on the flake
stream. It will have to be processed at temperatures sufficiently high for level - which is the only option on the current sink fraction - but on the
PET (above 250 °C), which is well above typical processing tempera- product level, as NIR is much more efficient there: both higher pro-
tures for PP, PS and PVC. cessing speeds and accuracy can be achieved since an object needs only
Fig. 1 describes the NIR sorting of the PVC and the effect on the a single scan instead of hundreds of particle scans. This would, how-
overall composition. The autosort flake low throughput NIR sorting ever, require a rethinking of the current industrial line: a PVC-positive
system positively selected out 20.6 wt% as PVC particles from the as- NIR scanner (complete with vibrating belt to distribute the different
delivered sink fraction. Of these, only 8 % were in fact PVC flakes. The waste evenly and pressurized air for controlled ‘shoot out’) would need
reject fraction hence contained 92 % of non-PVC particles, a large to be added before grinding. If this PVC is then also sent over a separate
number of false positives, a majority of which were determined to be grinding and washing line, it could even be recovered for PVC recycling
PET instead. Control on a lab FTIR showed that IR libraries tend to in the construction sector (Plinke et al., 2000).
show PVC as a potential ‘hit’ for many of the PET flakes, due to the In the longer term, it is quite possible that presence of PVC in
automatic choice of signature peak for identification. This constitutes a household waste will diminish by itself, as it is in line with Europe’s
severe material loss, which was deemed inevitable to allow for suffi- Plastics Strategy (European Comission, 2018) to harmonize the dif-
cient removal of PVC. Trials (not reported here) with less severe ferent types of plastics used in packaging and to phase out those plastics
scanning did not remove PVC to satisfying amounts. that are disturbing contaminators on the recycling process of mixed
This system sorted 79.4 wt% of the original sink fraction as PVC-free plastic waste. PVC for packaging applications would definitely be first
particles in the accept fraction, containing however still 2.1 wt% PVC- and foremost among these.
particles (in a batch of 500 samples) in the new mass balance of the Until then, the current sink fraction remains available in the market.
‘PVC-free’ sink fraction. The screening of the larger sample (990 g), For this manuscript, all further mention of the sink fraction pertains
however, reduced our estimation of the remaining PVC content to 1.0 to the currently sorted ‘PVC-free’ sink fraction with 1.0 wt% remaining
wt%. PVC content.
Given the industrial nature of the case study, it was most relevant to
work with the available state of technology. As such, optimization of
3.2. Technical quality of the sink fraction
this sorting pretreatment itself was not considered in-scope. Arguable,
secure setting of detection speeds and NIR camera could improve either
Table 2 summarizes the density and mechanical properties of the
the precision of PVC removal (more true positives on PVC) or reduce
sink fraction ‘as is’ and with the addition of 2 wt% compatibilizer SEBS-
the secondary residue (less false postives on PVC), but this would al-
g-MA.
most certainly go at the expense of processing speeds (tonnes/hour), as
The density of the ‘as is’ sink fraction is in the range of commercial
there is ever a trade-off between purity grade and recovery amount
PET densities and does not change significantly with the addition of the
(Morrish et al., 2010).
compatibilizer, meaning that if this mix were to be recycled again with
While the remaining amount of 1 wt% PVC is still significantly
density-based techniques, it would once more end up in the PET-rich

Table 2
values of density, tensile modulus Et, yield strength σy, strain at break εb and impact strength for the sink fraction (SF) and compatibilized sink fraction
(SF_SEBSgMA).
material density tensile modulus Et yield strength σy strain at break εb impact

[g/cm³] [MPa] [MPa] [%] [kJ/m²]


SF 1.31 ± 0.01 2519 ± 300 30.2 ± 4.9 2.76 ± 1.31 1.6 ± 0.5
SF_SEBSgMA 1.32 ± 0.02 2381 ± 150 29.6 ± 3.8 14.4 ± 12.1 5.2 ± 0.4

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K. Ragaert, et al. Resources, Conservation & Recycling 155 (2020) 104646

fraction. Somewhat surprisingly, strength properties (modulus and upper end/better for the compatibilized blend) concerning impact
yield strength) of the sink fraction are quite good and well within the strength. MPO is typically a recycled material (from the float fraction),
common range for virgin PET granulates (Equipolymers, 2014). Strain- which is typically used for garden furniture, terrace or wall panels. The
at-break is quite low for a thermoplastic polymer blend containing a lower stiffness (lower than virgin PP) is usually compensated by man-
significant amount of PP (typical values range between 50–150 % for ufacturing bulky products. We observe that the sink fraction is sig-
PP) and a rather large variation in the tensile properties is noted. nificantly stiffer than this MPO, so it could be used in similar applica-
However, this is typical for complex (recycled) polymer mixes (Hubo tion perhaps, but with thinner section. The addition of the (expensive)
et al., 2015), as tensile testing is quite sensitive to stress concentrators compatibilizer would only be warranted if the newly designed product
and local inhomogeneity; an unmolten particle will change the local is expected to be subjected to impact loading.
stress situation and cause modified deformation and failure behaviour.
This is a flaw to be taken into account when continuing with product 3.3.2. Product design: Greentile
design. The potential stress concentrators will also adversely affect the Based on the determined mechanical properties, it is decided to
impact resistance of the already quite brittle PET, as can be seen from develop a product where rigidity is required but at the same time the
the relatively low impact value of 1.6 kJ/m2. This makes the material critical load-bearing aspect of the product should be limited. The re-
unsuitable for products that are expected to be occasionally subjected to lative brittleness could be compensated by going for a slightly thicker-
sudden loads, like pallets or automotive parts. walled product, which will also mitigate the potential disturbance by
The addition of the SEBS-g-MA is seen to significantly improve the non-melting particles that could otherwise block the polymer flow in
properties related to toughness and ductility, namely strain-at-break the mould or be stress concentrators in the final product. Applications
and impact strength. Through compatibilization of the different frac- requiring a high strength/weight ratio (like transportation) are there-
tions present, the material is better able to disperse energy and forces. fore discounted, as the product will inevitably be heavier than a thin-
This will most likely occur between the PET majority phase and the walled counterpart. The sector of consumer products in electric and
second-largest PP phase. SEBS-g-MA is known to migrate to the inter- electronic equipment (EEE) is also discarded, as such polymers typically
face between these two components, where the SEBS backbone will require more impact resistance.
interact (dispersive forces) with the PP and the MA functional group For the sink fraction, the building & construction (B&C) sector was
will either bond or interact with polar groups of PET (Razak et al., determined as most suitable. The size of the products is often larger
2013). As SEBS is a rubberlike component, the overall blend will lose than other sectors and wall thickness often not critical. This gives en-
some of its stiffness. The noted reduction is not statistically significant, ough freedom to design the product to achieve the desired strength and
however, due to the large variations on the tensile measurements. durability. We aim for a relatively thick-walled product (6 mm) that is
subjected to small loads only. The thick wall section is meant to in-
crease strength and to buffer any unmolten particles. The product must
3.3. Design from recycling with the sink fraction
be suitable for mass production but not fall under bulk solutions (ty-
pically 100−300 mm thickness).
3.3.1. Product type from recyclate properties
All of these criteria come together in the Greentile product, a roof
From the characterization of the pretreated sink fraction, we can
tile for slanted green roofs on domestic residences or small sheds. An
estimate the behaviour of the material in a product and situate this
increasing popularity of green roofs is underpinning the market value of
previously untested blend with regard to other commonly used poly-
this product. Advantages of green roofs are including benefits for re-
mers, both virgin (PP, PP talc-filled, PET) and recycled (MPO) as shown
ducing air pollution in densely populated cities alone, alternative
in Fig. 2.
manner of cooling, contribution to the environment and the quality of
The properties of both the ‘as is’ and compatibilized sink fraction
life in many different ways (Blank et al., 2013). Roof tiles for flat green
fall within the broader range of virgin PET materials. PET is not often
roofs currently exist in the market and are often made from recycled PP
used as a resource for other than food packaging, so the comparison to
or MPO, as they have very limited load bearing function if any at all.
40 % talc-filled PP, which is commonly used in e.g. automotive or
Inclined green roofs are far more challenging, both from a construction
construction parts, is a more useful one. The sink fraction is somewhat
perspective (support, positioning, attachment, water management) and
weaker than 40 % filled PP, but in the same range (or even towards
in terms of material properties (sufficient strength for ‘hanging’ under
inclination and load variation dry-wet). The rooftile for inclined green
roofs in itself is innovative as a product and the required material needs
to be stronger than typical PP or MPO, while impact requirements are
limited, which makes the cheap ‘as is’ sink fraction (no compatibilizer
added) a suitable candidate.
The geometry of the new Greentile product is shown in Fig. 3, with
an indication of its most prominent features. The outer dimensions are
369 × 349 × 100 mm3, which is similar to common roof tiles, so that
one could replace a regular slanted roof with a Greentile roof without
having to adjust he support batten structure.
Inside the Greentile a grid of ribs (1) is placed, with three different
functionalities. Firstly, the grid serves to increase the stiffness and
strength of the rooftile, as well as its creep resistance. During the life-
time of the product, the Greentile is subjected to constant loading from
the substrate and vegetation, under which it is not allowed to fail. The
second function is water storage. The ribs form individual pockets
where water can be collected and contained. These water reserves can
be used by the vegetation during dryer periods.
Fig. 2. Stiffness/impact property balance of the sink fraction (SF), compatibi- The retaining wall (2) at the bottom end of a Greentile is meant to
lized sink fraction (SF_SEBSgMA) against common ranges for PET, PP, MPO and shore up the substrate and vegetation, even under high roof inclina-
talc-filled PP (Fox et al., 1997; Garbassi and Po, 2003; Lepoittevin and Roger, tions. This feature creates individual ‘shoring sections’ when placed on
2011; Maddah, 2016; Shubhra et al., 2013; Hubo et al., 2016). the roof, which means that one tile only needs to retain the weight of

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K. Ragaert, et al. Resources, Conservation & Recycling 155 (2020) 104646

Table 3
Summary of the resulting maximum stress (σ) and displacement (d) values for
FEM of four load cases. Conclusions are either OK (=Resulting stress is below
yield stress, no further action needed) or NOK (Resulting stress exceeds yield
stress, action needed).
Load case Inclination (°) d (mm) σ (N/mm²) Conclusion

1 15 1,0 33 NOK
45 0,9 53 NOK
55 0,9 57 NOK
2 15 0,9 20 OK
45 0,7 16 OK
55 0,6 13 OK
3 15 0,2 6,1 OK
45 0,4 6,3 OK
55 0,5 6,4 OK
4 15 0,9 20 OK
45 0,7 16 OK
55 0,6 13 OK
Fig. 3. design of the Greentile with marked features.

the substrate placed in that tile. This spreads the forces over the in-
dividual tiles, making it possible to optimize the amount of material
needed to produce one tile.
Underneath the retaining wall, a groove (3) is added to ensure
drainage of excess water during rainfall. The water is meant to cascade
from tile to tile, while draining via the substrate. This creates a buffer,
releasing the water slowly and steadily during pouring rains, ensuring
the substrate and vegetation are not oversaturated with water.
To protect the underlying roof from the vegetation roots, a double
edge is created with a root barrier (4). This makes it less likely that
roots would grow through the tiles, thus reducing the risk of roof
leakage and protecting the vapor barrier from root penetration.
A linear tolerance (5) of 20 mm was added to facilitate the place-
ment of the Greentile. This tolerance compensates for minor mistakes in
the placement of the support structure and makes it possible to adjust
the overall length of an entire row of Greentiles according to the length
of the roof structure. On the bottom of the product a reinforced rib (6) is
added. This is how the Greentile hooks to the underlying batten con-
struction, as the rib forms an anchor point for the tiles onto the wooden
battens. Finally, the Greentile was designed with large rounded corners Fig. 4. FEM analysis of load case 4, 15°. Maximum displacement (mm) is 0,9
(7). This facilitated the flow of the polymer, making the product easier mm around the contact of the foot.
to injection mould. More importantly, it prevents stress concentrations
in the product, that might give rise to brittle fracture. Also, a mass of temporary stresses up to maximum 20 MPa, still well below the yield
saturated substrate will be unable to grip in the sharp corners when it limit. The load of walking on the roof during installation (case 1),
expands during freezing weather. These big rounded corners provide an however, would be an issue. This is due to the fact that the area of the
upwards force when the mass would expand, protecting the tile from worker’s boot would only come into contact with the top surface of the
cracking. ribs and is therefore distributed over a very small surface area. This
issue worsens with increasing roof inclination. In practice, this could be
3.3.3. FEM analysis solved either by working in such a progressive fashion that workers
To ensure the durability and strength of the Greentile, FEM simu- needn’t walk on the ‘naked’ tiles or by first adding the substrate in the
lations were done during the design process. These simulations were system before walking on the roof. This would cause the load of walking
performed under various inclination and load situations including on the roof to be distributed over a larger surface area, a situation
walking, substrate mass, wind and snow. The results are summarized in which is overestimated (the newly deposited substrate/vegetation is not
Table 3. The results are shown in Fig. 4 for the load case 4 (15°), which saturated) by the problem-free case 2.
is representative for walking on a saturated substrate, with additional It was concluded that the Greentile was strong enough to go forward
wind and snow loads. It can be noted that the load from snow and wind with mould development.
is negligible to that of the walking human, as the resulting deflections
and stresses do not vary significantly from those obtained in case 2, 3.4. Production and evaluation of Greentile
with only the human walking as an added load.
It was concluded that the Greentile was strong enough to go forward The sink fraction was used for the production of Greentiles (scale
with mould development. All observed deformation remained below an 1:4), initially at temperature profile ‘260′. To be able to fill the com-
acceptable value of 1 mm maximum. For the static load situations (case plete cavity with the 80 T lab-scale injection machine, a combination of
2 and 3), the resulting stresses are considerably beneath the worst-case intrusion and injection moulding was used, which would be un-
yield limit of 25 MPa. The highest stress and deformation levels were necessary under industrial production circumstances. Therefore, one
observed for the low inclination situation (15°), which is the most un- should be careful with extrapolating our production experiences from
common roof inclination. From load case 4, it can be seen that walking the lab. In general, it was observed that the sink fraction is quite sen-
on the roof for maintenance will not cause the system to fail either, with sitive to processing temperatures. An initial temperature profile was set

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K. Ragaert, et al. Resources, Conservation & Recycling 155 (2020) 104646

at 260 °C, which is near to common temperatures for PET (265−300 virgin PP. The mixed household waste was considered as burden-free
°C). It was observed that the internal layer of the Greentile still con- up to the gate of the recycler. From there on, all process flow steps
tained unmolten particles, which upon control were identified to be (sink-float, different sorting steps on sink, drying, injection moulding,
PET. These unmolten PET particles hindered the effective flow of the etc) were included. In both comparisons, a clear environmental benefit
molten polymer stream, preventing a complete fill of the part in many was observed when producing the Greentile in the sink fraction. Even
cases and often blocking the nozzle and sprue. This effect is mainly with the energy consumption of the necessary decontamination steps
attributed to the specific lab-based production process itself. With and the relatively high contribution of injection moulding, this open-
conventional injection moulding, the polymer has a certain residence loop recycling of the sink fraction is preferable. Moreover, it allows for
time in the screw, while the previous part cools. In our lab setup, continued circularity of this challenging plastic waste fraction instead
however, the necessary preliminary intrusion step is quite fast, feeding of a one-time linear end in incineration.
the material directly into the mould. There is no stationary time in the While it would also be of interest to be able to compare the
heated screw and not all polymer is molten. A better flow of the molten Greentile to similar B&C products (be they in plastics or other mate-
polymer stream was achieved by widening the injection nozzle (to- rials), it is not possible to make a scientifically sound comparison. They
gether with the sprue), from just under 2 mm–9 mm in diameter. A cannot be compared to current green roof tile-based solutions, as in-
thicker passage insulated the heat better into the melt and if any par- sufficient public data is available regarding their material sourcing,
ticles do remain unmolten, they will be able to flow through. It was production process and geometry. They can also not be compared to
then possible to injection mould a satisfactory product. This specific existing rooftiles (mostly ceramic) for slanted roofs, as these do not
issue should be resolved when moving on to industrial production on a incorporate the green roof functionality and are therefore a different
larger machine, where conventional injection moulding can be applied. type of product.
As an alternative method to achieve better melting of all particles, a An exploratory market study of the Greentile concept was per-
trial was done at higher injection temperature (280 °C). Despites re- formed, defining the beach head target group, the market protentional
sulting in a more homogeneous melt, flashing was present on the sur- and the competitivity of the market. The beach head target group was
face of the entire Greentile part, mostly concentrated at the sprue. The set to be professional green roof installers. The potential market turn-
part showed a dark colour, had a brittle appearance and featured a over was evaluated at 2,6 million euro within Belgium, with increasing
homogenous melt with a distinct layered build, constituted of a foamed potential to go international. The business model used for this study
core and a brittle shell region, all features hinting at the presence of was based on an online resale platform combined with just in time
degradation and at the production of volatile components. It is surmised deliveries and waste (trimmings) collection to be used as raw material
that the remaining PVC content effectively degraded at these tem- for new Greentiles. The market was evaluated and was found to be a
peratures, causing degradation and devolatilization. Hence, the tem- low-competitive market. Only two companies are found offering similar
perature profile of 280 °C was abandoned. systems for inclining green roofs: the German based Optigrün
Produced Greentiles were used to construct a slanted green roof in a (Optigrün, 2018) system and the Groendakpan (Groendak, 2018) based
small-scale test setup. This was constructed with the traditionally used in The Netherlands. The Greentile system was evaluated to require a
wooden support battens, which serve as the anchors for Greentile retail price of €50/m² to be profitable, making it at least €12/m²
system. The inclination of the roof structure could also be changed cheaper than the closest competition.
between the very gentle case of 15° and the higher value of 45°; for the With regard to environmental benefits, it is not straightforward to
initial test this was fixed at intermediate value 25°. In Fig. 5 the process accurately compare the Greentiles to conventional rooftiles, as the
of installing the Greentiles can be seen. First the Greentiles are placed former serve more than just the function of covering a roof.
on the roof construction. This is done in a wave like pattern. Once the Nonetheless, an exploratory LCA was performed to compare the
Greentiles are placed on the test setup, substrate was added in the Greentile – as a construction product – to a conventional clay rooftile.
system (8−10 cm) and finally the vegetation carpets are rolled out. In this LCA the carbon footprint of the tile production was calculated.
The system was left to itself and the elements for three months. It For the Greentile, this was calculated according to the methodology
was set up in a sunny, unprotected position in an open grass field in described by Huysveld et al. (Huysveld et al., 2019). The carbon foot-
Ghent, Belgium. No water or nutrients were added before or during the print per kg clay rooftile was obtained from the ecoinvent v3.4 data-
trial period. After three months, it could be seen that the vegetation is base. Table 4 shows the results of the calculation, continuing from the
in excellent health and is in fact blooming (Fig. 5). carbon footprint per kg to an equivalent value for one square meter of
In a separate study (Huysveld et al., 2019), LCA was conducted on roof. This is calculated with the full size of the Greentile (not the scale
the Greentile, comparing the scenarios of (i) recycling the sink fraction model) and includes the effects of the recycling process.
into the Greentile versus incineration of the sink fraction and (ii) The largest contributor to the footprint of both systems is the pro-
Greentile production in sink fraction versus Greentile production in duction stage. From this exploratory calculation, the carbon footprint of

Fig. 5. Overview of the construction of the Greentile slanted roof. From left to right: construction of support battens, placement of roof tiles, filling with substrate,
adding of vegetation and greenroof after three months.

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K. Ragaert, et al. Resources, Conservation & Recycling 155 (2020) 104646

Table 4
Results of the comparative LCA between Greentile and conventional clay rooftiles.
Carbon footprint [kg CO2 equiv.] Surface size/tile [mm2] Mass/tile [kg] Mass/m2 [kg] carbon footprint/m2 of roof [kg CO2 equiv.]

Greentile 0,687 369*346 1,9 22,5 15,46


Clay rooftile 0,358 310*252 2,8 45,0 16,11

the Greentile is very similar to the conventional clay rooftile. However, hampering recycling processes (will) have been replaced or phased out’.
this does not take into account the benefits obtained by giving the re- In the meanwhile, Design from Recycling is a clever potential so-
cycled plastics an alternative destination to incineration. lution for the sustainable valorization of these materials.
Furthermore, some additional critical notes deserve to be made with
regard to these comparison, being that (a) the comparison only takes 4. Conclusions
into account production and not transportation (wherein the clay tile is
heavier), (b) the calculation assumed a single-cavity injection moulding In this research, the complex sink fraction of post-consumer
of the Greentile, which is less energy-efficient than multi-cavity injec- packaging waste has been extensively characterized. This waste stream
tion and (c) the added function of greenroofing is not yet included. is typically bound for incineration. It was found to be a PET-dominated
As such, we expect that a more elaborate comparison would result mix, contaminated with nearly 10 wt% PVC and some non-ferrous
quite decisively in favour of the Greentile. particles. Sorting steps were undertaken to remove these troublesome
The relevance of the sink fraction as a currently untapped resource contaminations, after which the Design from Recycling strategy was
for plastics is high: it is a sizeable share of the mixed post-consumer applied to develop a suitable product to manufacture in the sink frac-
plastic waste and current end-of-life options are usually incineration. tion. This product, the so-called Greentile, is a robust construction
Furthermore, the amount collected of such waste is expected to increase element for slanted green roofs. FEM analysis was conducted to ensure
in future as ever more ambitious collection and recycling goals are to be sufficient strength of the design and a prototype mould was made for
realized (European Commission, 2018). Some countries, like Belgium, the production of a test series of Greentile products. A small greenroof
are currently expanding their kerbside collection systems to include all was successfully built and evaluated with these Greentiles.
postconsumer packaging waste (Coberec-Go4Circle, 2018), while other With regard to the processing of the sink fraction, both the complex
countries like The Netherlands and Germany already have this in place. composition and the remaining PVC content of the mix remain a point
Additionally, the separate collection of plastics at recycling parks of attention and might inhibit large-scale adoption of this material.
steadily increases as well. This too, is a complex mix of all common Nonetheless, the Greentile is a case study of how even challenging
plastics. recycled plastics can be valorized. It is the first known valorization –
It will depend largely on the sorting/recycling systems in place how other than incineration – for this challenging plastic waste.
this potential sink fraction will be handled. On the one hand, there are
those recyclers who rely on a fully mechanical separation line, yielding Acknowledgements
the ‘float’ and ‘sink’ fraction as described earlier (Ragaert et al., 2017).
On the other hand, there are those current systems for food packaging The authors were financially supported by Flanders Innovation and
sorting which are mostly NIR-based and to date focus on the recovery of Entrepreneurship Agencywithin the TETRA-IWT project “Design from
PET bottles (3 colours), HDPE and sometimes PP as well (Ragaert et al., Recycling” (150151). The authors wish to acknowledge dr. Ulphard
2017). Specifically for the current roll-out of the expanded (the so- Thoden van Velzen (Wageningen University) for his contribution to the
called P + MD) kerbside collection in Belgium, it has now been spe- extensive NIR analysis, MSc Karen Van Kets (Ghent University) for her
cified that sorters receiving the mixed plastic waste must sort out the help with the analysis of the materials, mr. Marcel Moerman (Ghent
plastics into 11 different fractions, all of them aimed at being as much University) for his assistance with the mould design, mr. Mustafa Erkoç
as possible mono-materials (FostPlus, 2019). The sorting companies (Ghent University) for his assistance with the injection moulding and
involved are currently adapting their existing sorting lines, amongst the companies ECO-oh! and SUEZ for the materials and discussion.
other to sorting out also PET trays, PS and foils (Indaver, 2019).
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