Proceedings of TMCE 2014, May 19-23, 2014, Budapest, Hungary, Edited by I. Horvth, Z.

Rusk
Organizing Committee of TMCE 2014, ISBN 978-94-6186-177-1
23
CONTROLLED POLYMER RECYCLING AND DEGRADATION A TUTORIAL
Gyrgy Bnhegyi
Department of Advanced Materials and Processes
Bay Zoltn Nonprofit Ltd. for Applied Research
Hungary
gyorgy.banhegyi@bayzoltan.hu



ABSTRACT
Polymer materials became an indispensable part of
our life in the 20th century and they will surely be
with us in the 21st century as well. They are, and will
be, indispensable because of their advantageous
properties, such as low density, relatively low
specific energy consumption during production, easy
and large scale processability, but they also require
keen attention because of their environmental effects,
such as permanence, slow degradability, potentially
harmful additives etc. In this tutorial only a few
relevant aspects of this complicated problem can be
touched, and even those very briefly: the origin and
distribution of plastic waste; main directions of
utilizing/recycling/disposing this waste; recycling of
plastic packaging waste; electrical and electronic
waste; automotive waste; commingled plastic waste;
thermosets and elastomers; the inter-relation
between recycling and design; pros and cons of
controlled degradation; controlled photo-oxidative
degradation; bio-degradation and finally the
possibilities of a sustainable polymer technology.
KEYWORDS
Recycling, plastics, environment, thermoplastic,
thermoset, rubber
1. INTRODUCTION
Nowadays it is fashionable and not only in the
green circles to blame plastics for almost all
environmental problems. Philippics against PVC can
be read and heard everywhere, although the simple
question: what would the environmentalists do with
the huge amounts of chlorine obtained as a byproduct
of caustic soda production is rarely answered (in fact,
the problem is usually not even recognized). Some of
the hardliners would answer: you should not produce
caustic soda either. I wonder how they could tolerate
each others smell without using soap which
requires caustic soda. But let us not be sarcastic:
plastic waste is a huge problem that should be
handled carefully [1]. Waste should be considered as
a potentially valuable resource instead of simply
being a burden [2]. Before seriously considering the
elimination of plastics, the economic, social and
other costs of replacement should also be considered.
Simple negation of a technology may sound
attractive but a real answer should always discuss the
consequences. If we remain at the level of political
propaganda, the solutions will not survive the next
political cycle.
Due to the complexity of the problem, which is not
only technical, but also economic and societal in
nature, and to demonstrate the actuality of the
discussions related to this topic, only a minor part of
the references used in compiling this tutorial were
taken directly from the technical literature, most of
them come from various surveys made by authorities,
websites etc. No comprehensive review can be
attempted at this length, therefore only brief
comments on selected examples can be offered.
Nevertheless I hope that at least the versatility of the
various approaches and the inter-relatedness of the
emerging problems can be presented.
2. BASIC NOTIONS
Before starting the discussion of plastic waste, some
very basic notions should be clarified. Plastics got
their name from the fact that they can be shaped
relatively easily in the molten state by highly
efficient methods (such as injection moulding or
extrusion) and maintain their shape after cooling.
This basic property is closely related to their
molecular structure, i.e. to the fact that they are
composed of long, relatively flexible, mostly linear
molecules - in contrast to low molecular materials.
Upon melting low molecular materials (including
metals and ionic solids) form low viscosity liquids,
mostly described by Newtonian viscosity, while
polymers tend to exhibit visco-elastic properties both
in molten and in solid states.
Another important difference from low molecular

24 Gyrgy Bnhegyi
solids and liquids is that in plastics the molecules are
rarely uniform. These polymer chains (repetition
units are called monomers) are of different length,
therefore the molar mass exhibits a distribution
characteristic of the polymerization method. This
molecular mass distribution has far-reaching
consequences on the viscosity of the polymer melt
(essentially determined by the average molar mass),
while the shape and breadth of the distribution curve
influences such phenomena as the frequency or shear
rate dependence of the viscosity or the melt strength.
Not only the molar mass values of the various
polymer molecules are not uniform, but also the
molecules may exhibit various polymerization
defects. One typical defect is branching, which may
be short chain branching (if the length of the branch
is negligible with respect to the longest linear chain)
or long chain branching (if they are comparable).
Branching means that at least some monomers are
trifunctional and not bifunctional. Trifunctional units
may be added to the monomers consciously or they
may be formed by chance as a polymerization defect.
If the branches are long and if the concentration of
the branching units reaches a critical concentration
the polymers becomes a gel, i.e. a non-flowing
network is formed.
On this basis so-called thermoplastic and thermoset
materials are distinguished: thermoplastics contain
linear (or slightly branched) macromolecules where
the branching density does not reach the critical
value necessary for gelling. Thermoplastics can be
re-melted, which makes their recycling easier. Even
linear macromolecules can be rendered thermoset by
crosslinking reactions (e.g. vulcanization, radiation
crosslinking), typically used in rubbers. Typical
thermoset resins are, however, relatively low
molecular, easy flowing liquids which become
multifunctional during the so-called curing reaction.
Once the network is formed, it cannot melt (unless if
it is based on physical crosslinking or reversible
chemical bonding), only degrade at high temperature
(hence the name: thermoset).
Plastics are typically amorphous (lacking long-range
order), exhibiting one typical transition temperature:
the glass-rubber transition (Tg). Unlike melting, it is
not a thermodynamic transition (although some
believe that a so-called second order transition exists
close to Tg), but a relaxation transition, where the
quasi-solid amorphous material becomes a visco-
elastic melt. (At even higher temperatures the melt
tends to become more purely viscous). Some other
plastics exhibit two, intimately mixed phases:
crystalline and amorphous. The crystallites are
typically very small and the degree of crystallinity
may strongly depend on the thermal and shear
history. Such, so-called semi-crystalline polymers
exhibit two transitions: the glass-rubber transition
(Tg) and melting (Tm). Generally semi-crystalline
polymers exhibit higher thermal resistance, although
their processing may become more complicated
because of secondary crystallization.
It should be noted that industrially available plastics
are much more than simple polymers, they are rather
compounds, usually intricately formulated multi-
component materials. Even plastics containing only
one kind of polymer need additives that render them
well processable and stable under e.g. outdoor
conditions. Other plastics are blends, i.e. mixtures of
more types of polymers, still others contain organic
or inorganic reinforcements or functional fillers. This
complexity makes the recycling activity more
complicated as an additive designed for a certain
plastic compound may be detrimental for another
purpose. This emphasizes the necessity of selective
collection and/or separation of various plastics from
the waste stream.
A last, practically important classification of plastics
is the distinction of so-called commodity plastics
(polyolefins, vinyls and styrenics nowadays also
PET is added here), engineering plastics and high
performance polymers (the latter are sometimes
divided into high temperature and very high
temperature grades). Therefore the commercially
available polymers are frequently represented by a
pyramid, consisting of two halves: amorphous and
crystalline polymers. The broad base of the pyramid
is the family of commodity resins.
The next stage is the group of engineering plastics
(such as polyesters, polyamides, acrylics, polyacetal
etc.), while the top of the pyramid include high
performance engineering plastics. The higher we
climb on the pyramid, the higher are the temperature
resistance values and the price and the lower the
production volume. The decrease of production
volume is faster than linear: almost 75% of the EU
plastic consumption in 2011 belonged to the
commodity plastics. Almost 40% of the total demand
was used by the packaging industry, about 20% by
building and construction, 8% by the automotive
industry and 5% by the electrical and electronic
industry [3] (see Figures 1 and 2).

CONTROLLED POLYMER RECYCLING AND DEGRADATION A TUTORIAL 25

Figure 1 Plastic consumption in the EU in 2011 by
plastic types (Source Plastics Europe)

Figure 2 Plastics consumption in the EU in 2011 by
applications (Source Plastics Europe)
3. PLASTIC WASTE ITS ORIGIN AND
DISTRIBUTION
No wonder then that the majority of plastic waste
also comes from the commodity plastics. Some
important sources plastic wastes are listed below [4]:
Plastics conversion, processing waste, scrap, (in-
house)
Packaging waste (selectively collected)
Post-consumer waste (selectively collected)
Municipal solid waste
Agricultural waste
Construction and demolition waste
Automotive waste (end-of-life vehicle, tires)
Electrical and electronic waste
While about 45% of the industrial waste is recycled,
and only 10% ends up in the landfill, about 70-80%
of the domestic plastic waste is incinerated. The
composition of municipal solid waste (MSW) may
vary from country to country, even from town to
town, the definition of plastic waste is also
somewhat ambiguous in various statistics (whether
rubber, man-made fiber or paint is included or not),
but on the average 10-15 wt% of the MSW is plastic
[5] (see e.g. Figure 3). The distribution of plastics in
the waste closely resembles the production rates [6]:
about 81% of them belong to the commodity plastics
(see Figure 4).

Figure 3 Distribution of the municipal solid waste in the
USA in 2010. Source: www.eschooltoday.com/
waste-recycling/sources-of-waste.html

Figure 4 Distribution of plastics in the municipal solid
waste. Source: www.naturalstateresearch.com/
ProductsPage.html
4. WHAT CAN BE DONE WITH PLASTIC
WASTE?
There are more levels and possibilities of recycling
[7]. The ideal is mechanical or material recycling
where the waste is mechanically ground (reclaim,
regranulation, scrap reuse). It is feasible with
production waste or with selectively collected plastic
waste (e.g. packaging waste). It is less efficient with
commingled plastic waste (fractionation is
necessary), even less with municipal solid waste. The
main limitation of this technology is the
immiscibility of most thermoplastics with each other
and the contamination (partial degradation, soil,

26 Gyrgy Bnhegyi
foreign particles etc.). Upgrading of plastic waste,
where the original properties are reached or even
exceeded is very rare downgrading is much more
frequent. It means that in the majority of mechanical
recycling technologies the original application is not
feasible, some less demanding products should be
sought. Chemical recycling means that waste is
converted into other, valuable raw materials by
depolymerisation [8], cracking, hydrogenation,
hydrolysis (in the case of polycondensation
polymers), solvolysis (PUR), peptization (rubbers).
Biological recycling by bacteria and enzymes means
conversion of plastics to lower molecular products
such as biogas, biomass, and so on. This possibility is
very much limited with fossil based plastics. It can be
used, however with so-called degradable plastics.
Energy recovery, i.e. direct burning or co-firing in
cement kilns, blast furnace, in combination with
other fuels is an obvious option but one should take
care of the potentially dangerous byproducts. (This is
true for municipal waste incineration as well). One
cannot emphasize enough the responsibility of the
industrialized states vs. the developing countries:
illegal waste trade, pollution, exporting the problems
should be prevented by all means!
Figure 5 shows the flow chart of new and waste
plastic streams in the EU from a survey made in 2010
[9]. The European Union issued several directives
related to the waste problem, e.g. the EU Directive
94/62/EC of 20 December 1994 on packaging and
packaging waste, which prescribed 22.5 wt%
recycling by 2008, or Directive 2008/98/EC which
demand 50% recycling by 2020. Other relevant
directives are 2012/19/EU on the electronic and
electrical waste or the end of life vehicle directive
2000/53/EC, which will be discussed later.
The question, whether material recycling or energy
recovery is more economic or useful, has been
investigated for a long time [10]. From the viewpoint
of energy utilization alone, incineration should be
preferred. Such questions are, however, more
complicated than that and the whole complexity of
problems, including environmental pollution and
social costs should also be included in the balance.
The answer always depends on the technology used
therefore decision should be supported by constantly
updated calculations. This will be discussed in some
length in relation to LCA (Lifecycle Analysis)
methods.
4.1. Plastic packaging waste
In view of the large amount of plastics used for
packaging, the importance of this kind of waste in
environmental pollution and the relatively good
chance for collecting at least a substantial part of this
kind of waste before getting into the MSW stream
plastic packaging waste is a good target of recycling
[11], [12]. Recycling of agricultural plastic waste (at
least that of agricultural films) overlaps partly with
the technologies used for recycling plastic packaging
waste (films), although it has specific features due to
the different nature of contamination and to the
differences in the additive package. (We will return
to this latter problem when treating the controlled
degradation problem).
The majority of packaging scrap is in the form of
films: bags, sacks, various kinds of food packaging
(food contact and non-contact grades as well), shrink

Figure 5 Import, consumption, recycling and export of new and waste plastic in the EU based on a 2010 study [9]

CONTROLLED POLYMER RECYCLING AND DEGRADATION A TUTORIAL 27
films, stretch films, cling films and so on. There are
problems even with selectively collected films: one
major problem is that most up-to-date films are
multilayer structures, where, in addition to
polyolefins (LDPE, LLDPE, HDPPE, olefin
plastomers, PP) typically there are other layers as
well (such as polyamides, tie-layer resins, which are
typically olefin copolymers with polar co-monomers
or grafts). Another possible problem is contamination
[13], [14] by greases, other organic components, soil
etc. A third problem is that even various types of
polyolefins are not necessarily compatible [15] (they
are, in fact, normally incompatible) which means
severe downgrading in properties (especially in
elongation at break) if simple melt mixing is applied.
The use of compatibilizers (mostly block
copolymers) may be of some help. A further
complication may come from composite laminates,
such as plastic/paper, plastic/aluminum or
paper/plastic/aluminum multilayer packaging. These
are very modern and highly functional, but the
components cannot be easily separated from each
other, thus hampering recycling.
In addition to films other plastic packaging materials
are available in the form of injection molded or
vacuum or thermoformed boxes, cups, blow molded
containers or bottles. Boxes and cups are usually
made of PE, PP or PS, while bottles and containers
from HDPE [16] or PET (PVC is much less used
nowadays for this purpose).
Collection of selective packaging waste should begin
at the retail stores where e.g. a large portion of shrink
and stretch films can be recollected after product
delivery. Other parts of packaging waste can be
collected selectively by the households. Nowadays
this selective collection is mostly limited to PET
bottles. In less developed countries the majority of
plastic waste can be found in MSW. If it goes to
landfill, it causes problems; if it is incinerated, at
least the energy content is recovered.
A typical recycling line [17] which can be used not
only for plastic packaging waste, but also for other
plastic scraps is shown in Figure 6. The milled waste
is first washed (cleaned, decontaminated), the various
additives are added and finally the mixture is
compounded and granulated. Regranulation lines
usually contain easily changeable melt-filtering units,
as fine solid particles clog the filters relatively
frequently in spite of the initial washing step. In
post-consumer waste the polymer molecules are
somewhat degraded (oxidized and/or the average
molecular weight is reduced). Oxidation may be
accompanied by discoloration and the antioxidants
and heat stabilizers are typically depleted. Therefore
additional stabilization is necessary. Contamination
level should be kept low if the recycled polymer is to
be used again for food packaging. Leachate level
should be very low. The hazards can be significantly
reduced if the recycled plastic is used in multilayer
films again where the recyclate is in the central layer
and the outer layers are made of virgin resin. Co-
injection and multilayer blow molding are similar
strategies in other applications.
Molecular weight reduction in post-consumer PET
bottle recyclate may be quite serious. This may be
one reason why the majority of PET recyclate is used
for fiber purposes and not for bottle production (see
Figure 7). Fiber spinning requires much more fluid
plastic grades than bottle production.
If PET recyclate is to be used for the original
purpose, chain-extension and recrystallization
processes are made [18]. In recycled PET bottle
manufacturing the multi-layer approach with central
recyclate layers is also widely adopted.

Figure 6 Flow chart of a typical plastic waste regranulation line after [8].

28 Gyrgy Bnhegyi

Figure 7 Consumption of PET recyclate for various
purposes. Source: University of Cambridge,
ImpEE project, Topics/Recycling Statistics
4.2. Electrical and electronic waste
In our consumer society the lifecycle of up-to-date
electronic equipment became very short, new
communication and data storage technologies
become completely obsolete within 5 years together
with the hardware. This is accompanied by an ever
growing amount of electrical and electronic waste,
where not only the amount is alarming but the
hazardousness of some components. Presently at
least two directives deal with this problem is the EU:
the WEEE Directive 2002/96/EC and the RoHS
Directive 2002/95/EC. Most industrial countries try
to regulate the selective collection of electronic waste
by the manufacturers and the vendors. This is
important because of both the valuable and
hazardous materials contents. The electronic waste
contains 49% metals, 33% plastic, 12% comes from
cathode ray tubes (which may diminish with LCD
and other displays), the rest contains different
materials [19].
According to the same source in 2005 in the US
about 56% of the WEEE plastics fraction was HIPS,
20% was ABS, 11% was PPE (poly-phenylene-ether,
which, together with HIPS constituted a popular
blend, called Noryl), while the residue (13%)
contained other polymers. Nowadays probably the
PC content is higher due to the widespread use of
PC-ABS alloys, but essentially E-waste plastic
fraction is a strongly mixed powder of engineering
plastics. The most important fraction of electronic
waste is that of metals: some precious metal (Au, Pd,
Cu, Ni, Sn, Pb) components are present there in
significantly higher concentration than in natural ores
[20], and can be recovered after mechanical
separation followed by classical or hydro-
metallurgical and electrochemical processes. It is
quite possible that it will be less expensive to recover
some metals from the E-waste than from natural
resources.
The plastic fraction is less valuable (mainly because
of the necessity of component separation and
contamination), nevertheless the constituents a
relatively expensive engineering plastics. The E-
waste recycling rate increased from 10% in 2000 to
24.9% in 2011 [21]. The E-waste problem is not
limited to the USA or the EU countries, Asian
countries face the same problem [22]. Separation and
reprocessing of the E-waste plastic fraction are
somewhat similar to those technologies used in the
processing of the automotive shredder plastics
residue. Material recycling is very much limited by
the technical difficulties of component separation,
controlled decomposition into low molecular organic
compounds, incineration or co-firing are better suited
to this kind of waste. Plastics of different chemical
composition may be separated from each other by
various techniques, based on density, wetting or
triboelectric behavior (see the next section). E-wastes
are problematic because of the presence of
potentially hazardous components: most importantly
halogenated flame retardants, halogenated
hydrocarbons (coolants in refrigerators and air
conditioners), and various kinds of batteries (e.g.
lithium ion batteries).
This latter problem is dealt with by the RoHS
directive, which limits the use of halogenated flame
retardants, Cr(VI) based compounds, lead based
solder materials etc. The presence of printed circuit
boards based on thermosets (mostly epoxies)
complicates recycling further which will be
discussed in a later section. Prescribing the duty of
product collection by the manufacturers and vendors
can be easily circumvented by non-EU resident
companies. This is a general problem of the
consumer society: legislation always lags behind the
problems. Alleviation of the E-waste problem is also
possible by careful design, which will also be
touched briefly in a later section.
4.3. Automoti ve waste
In spite of the slowdown caused by the 2008
economic crisis, production and replacement of older
automobiles by the companies and by the population
results in a heavy environmental burden. In order to
reduce fuel consumption and CO2 emission the
portion of plastics used in new car models increased
continuously (see Figure 8).
Similarly to the E-waste, again plastics are the least

CONTROLLED POLYMER RECYCLING AND DEGRADATION A TUTORIAL 29
valuable components of the waste. Therefore great
efforts are made to recover steel and other non-
ferrous metals and the big problem is the economic
and useful reprocessing of automotive shredder
residue (ASR). As the so-called End-of life vehicle
(ELV) 2000/53/EC prescribes 85% reuse and
recovery of ELV by 2006 and 95% by 2015 plastic
fractions must be dealt with. The average
composition of the ASR is shown in Figure 9, taken
from a case study in Denmark [24]. Although the
margins vary widely, the organic fraction is
substantial.
The ferrous part is separated by magnetic field, while
the rest is mostly sorted based on their density
differences [25], [26]. Non-magnetic separation
technologies include trommel (size) separation,
vibration sieving, air classification (cyclons), sink
and float, manual sorting, on-line spectroscopy
assisted separation, eddy current separation and
triboelectric separation. The term sink and float
covers methods based on both wetting (froth
flotation) and density differences. If using organic
liquids (which are less tolerated nowadays for
environmental reasons) selective partial swelling of
various plastic grades can be utilized to increase
density differences. Due to the difficulties involved
in plastic separation one may think of burning the
organic residue, which has its own problems: high
humidity content (2-25%), relatively high inert
content (5-40% - resulting in slag formation), widely
varying and relatively low heating value (13-25
MJ /kg comparable with that of wood but much less
than that of pure polymers, coal or oil). Co-
incineration with municipal solid waste or sewage
sludge is also possible, but the presence of acidic
gaseous products and heavy metal contamination in
the dust requires attention. Pyrolysis in reductive
atmosphere (CO, CO2, H2 mixture formation) is also
possible.

Figure 8 Average material consumption for a domestic light vehicle, model years 1995, 2000, and 2009 (Source:
Wards Communications, Wards Motor Vehicle Facts and Figures, 2010Detroit, MI, 2010, pp. 65). The
picture is taken from a study made for the National Highway Traffic Safety Administration, USA [23]

Figure 9 Average composition of automotive car shredder residue, taken form [24]

30 Gyrgy Bnhegyi
Instead of describing a wide variety of technologies,
here we briefly refer to a PhD Thesis written by
Bodzay, parts of which are published internationally
[27-29] in which a density based fractionation
method is described for ELV-ASR fraction assisted
by on-line spectroscopic methods and various
possibilities for upgrading (e.g. flame retardant
addition, mechanical upgrading by layered composite
formation or transformation to carbon nanotubes by
laser pyrolysis in the presence of silicate additives)
are suggested. Essentially the following groups of
fractions can be treated as independent raw material
sources: <0.92 g/cm3 essentially PP, 0.92 g/cm3<
<0.97 g/cm3 PE contaminated by PP, 0.97
g/cm3< <1.00 g/cm3 filled PP, 1.05 g/cm3<
<1.30 g/cm3 PS + ABS, 1.3 g/cm3< <1.4 g/cm3
mixed. The almost pure polyolefin fractions (the
first group, about 20 wt% of the total) could be used
for upgrading (addition of stabilizer, reinforcement
and flame retardant), the slightly filled/
mixed/contaminated fractions (PE+PP, PS+ABS) for
less demanding applications, while strongly mixed
fraction as an asphalt additive or can be processed
further by pyrolysis. Broader range of the fractions
can be used even for upgraded products if sandwich
structures are also allowed, but that limits the range
of available processing technologies (as e.g.
compression molding).
An early economic analysis of the ELV directive [30]
investigated the effect of increased recycling targets
of 2015 on the global warming potential of recycling
vs. dumping but, due to some lacking data the wide
estimated margins do not allow drawing an
unambiguous conclusion.
4.4. Commingled plastic waste
One should distinguish commingled waste in
general and commingled plastic waste in
particular. The first term is used for single stream and
dual stream municipal solid waste where in the latter
case glass is separated, while the second term is used
separated plastic wastes where various kinds of
polymers occur together. The general problem with
mixed plastics recycling is the incompatibility of
most polymer pairs. Compatibility can be used in
the strict, thermodynamic sense and in technical-
practical sense. In the thermodynamic sense, because
of the very low mixing entropy only those polymer
pairs are miscible which exhibit exothermal mixing
(specific interactions). Such pairs are very rare. In the
practical sense two polymers are called compatible
if they form a macroscopically homogenous melt if
mixed in the molten state and produce acceptable
mechanical properties after cooling. Such pairs are
less rare which can be used as blends (e.g. ABS,
HIPS, ABS/PC blends, Noryl) even though their
microstructure reveals the presence of phase
boundaries. Properly distributed heterophase may
even increase the impact strength of the blend by
stopping crack propagation.
The stability of fine polymer/polymer dispersions
may be improved by adding special block
copolymers as compatibilizers, which accumulate at
the interfaces of two phases, or by using reactive
extrusion. In the latter case slight peroxide or other
modifier addition initiates chain breakage and
recombination of dissimilar polymer chains, which
essentially means in situ block copolymer
formation at the interface, which is the most effective
way of compatibilization. All this is easier said than
done, however, and it requires all skills of
experienced compounders to achieve the optimum
composition and morphology. Differences in
viscosity, color, filler content, stabilization, degree of
degradation, presence of elastomeric components etc.
all complicate reprocessing into useful product. Low-
end applications (e.g. extrusion certain kinds of
plastic lumber profiles) were attempted with more or
less success. Downgrading is almost inevitable.
Another problem, which long prevented the
processing of mixed plastic waste was the potential
presence of PVC. Handling the PVC problem in
mixed plastics recycling [31] has long been
investigated, as PVC begins to degrade and lose HCl
at temperatures which are customary processing
temperatures for other components of the mixture.
This early degradation is accompanied by strong
discoloration. If relatively pure PVC waste can be
collected (e.g. window and door profiles, pipes, cable
insulation, packaging materials), they can be
regranulated by themselves. In view of the
complicated formulation of PVC-s (both
unplasticized and plasticized ones) this is a delicate
task. The mechanical recycling of PVC waste in the
European countries has been reviewed by many [32],
and especially good results are achieved for window
profiles collected from demolition waste. If PVC is a
minority component in mixed plastic waste, its
content can be reduced by triboelectric separation or
by forced PVC degradation in a preliminary
extrusion step, where the majority of HCl is removed
and absorbed by bases.
Commingled plastic waste can also be reprocessed

CONTROLLED POLYMER RECYCLING AND DEGRADATION A TUTORIAL 31
by pyrolytic technologies. This broad term involves
various technologies, as [33]
hydrous pyrolysis (steam cracking) at 300-350 C
and at relatively low pressure (<12 MPa),
resulting in light hydrocarbons
hydrothermal liquefaction at 300-350 C and 12-
20 MPa, resulting in an aqueous slurry of liquid
hydrocarbons
anhydrous pyrolysis above 350 and above 12
MPa pressure, resulting in a whole series of
cracking products (gas, oil, char). This is the best
with polyolefin waste.
In case of incineration or co-firing the amount of
halogenated, nitrogen and sulfur containing
residues in the waste should be reduced to avoid
environmental pollution or basic slag formers
should be used.
5. THERMOSETS AND ELASTOMERS
Crosslinked polymers: thermosetting resins and
vulcanized elastomers (rubbers) are notoriously bad
targets of recycling, as they cannot be melted but
undergo thermal degradation on heating.
Thermoset resins are much lower in production
volume than thermoplastics, but (mainly due to their
thermal stability) they are indispensable in some key
areas (e.g. transport, E+E sector, aerospace, military).
Most thermoset composites contain a significant
amount of reinforcement (glass, carbon or other
fibers), the majority of the matrix resins are
polyesters (66%), epoxy resins (23%), the rest (11%)
includes all other resins as phenolics, amine resins,
vinylesters, urea-formaldehyde resins, thermoset
polyurethanes etc. [34] Polyester based composites
include SMC (sheet molding compounds), BMC
(bulk molding compounds) widely used by the
transport industry. Pultruded profiles and fiber
reinforced laminates are also important. Composite
and thermoset recycling methods [35]-[37] recycling
of plastic composites (including thermoplastics and
thermosets) [38] have been widely reviewed. One
possible way of utilizing thermoset composite waste
is grinding into fine powder and using the product as
inactive filler in other thermoset composites, in
thermoplastic composites or in rubbers. This means,
however, inevitable downgrading of the reinforcing
properties of the fibrous component, as continuous
filaments are transformed into chopped or even
milled fiber with much less reinforcing activity.
Additionally the surface of ground composite powder
is inactive therefore surface treatment may become
necessary if better properties are to be achieved.
Recovery of the reinforcing fibers may be considered
if the matrix is thermally or chemically decomposed.
It is feasible only for carbon reinforcement which is
expensive enough to warrant such a complicated
procedure. Anyway milled, chopped or pelletized
carbon fibers can be recovered form thermoset
composite waste with about 90% of the original
properties retained. Tertiary recycling of SMC into
fuel [39], [40] is possible, as well as solvolysis by
supercritical water or methanol, thermolysis and
gasification [41] into useful chemical raw materials.
These methods are similar to those described for
automotive shredder residue, E-waste plastic
fraction, mixed plastic or municipal solid waste,
shown earlier. The use of supercritical fluids for
matrix degradation is especially interesting, as e.g. in
supercritical water several reactions are extremely
fast even in the absence of catalysts.
Traditional chemical decomposition methods have
also been described (e.g. nitric acid for epoxy resins,
aminolysis for polyesters, glycolysis for thermoset
polyurethanes, see ref. [36]) which may be useful in
some applications, e.g. glycolyzed PUR wastes can
be re-used as polyols in new PUR formulations. In
principle thermoset composites may be replaced by
thermoplastic ones (e.g. LFT long fiber reinforced
thermoplastics, where the length of the fiber is equal
to the pellet length or even continuous fiber
reinforced thermoplastic profiles, mats), which can
be (in principle) fully recycled while retaining a
considerable portion of the reinforcing properties.
Due to the thermoplastic nature of the matrix,
however, the thermal resistance of such composites is
much more limited than that of thermoset
composites.
Rubber recycling is very important because of the
huge amounts of automotive tire wastes produced
every year. Dumping of waste tire is forbidden in
most industrialized countries, burning is severely
limited by laws, therefore material recycling is
necessary. Tires are, however, much more than
rubbers, they are complicated composite structures
containing textile, metal and rubber components. Tire
waste is not uniform in composition, several different
kinds of rubbers are used for this purpose (natural
rubber, styrene-butadiene rubber, nitrile rubber, butyl
rubber etc.). First the non-rubber components must
be separated and the residue is transformed into
crumb rubber by mechanical or e.g. water-jet
milling. Basic principles of rubber recycling have

32 Gyrgy Bnhegyi
been widely described in simple terms [42]. The
softness of elastomers limits the size and efficiency
of grinding.
Using room temperature grinding relatively coarse
crumbs are obtained, while cryogenic grinding
allows the production of sub-millimeter particles.
Even the latter are, however, macroscopic in
comparison to normal fillers with a typical diameter
of 1-10 microns. Crumb rubber can be compounded
into fresh elastomer, followed by vulcanization, it
can also be used in the formulation of thermoplastic
elastomers [43], or mixed with various
thermoplastics, as e.g. HDPE and nylon 6/10 [44].
Crumb rubber is a useful (but not cheap) additive for
asphalt in elastic pavements or in the top layer of
highways. Deposition taxes, however, may influence
economic considerations. The problem with crumb
rubber fillers in thermoplastic or in elastomeric
compounds is the same which we had to face in the
case of milled thermoset composites: the surface is
inactive the matrix-filler adhesion is low. It means
that either we limit ourselves to low-end applications
(e.g. rubber mats, vibration or sound absorbers etc.),
or we have to apply expensive post-treatment to the
crumb rubber surface. Another possible route is the
breakdown of the network into flowable sub-units
using so-called peptizing agents [45], which act
physically (as e.g. metal soaps) or chemically (thio-
compounds). High temperature steam or supercritical
water can also be used for the partial (or complete)
breakdown of rubber networks. These peptized
rubbers can be processed more easily into
elastomeric or thermoplastic compounds than crumb
rubber, but their production is more expensive.
Problems associated with rubber recycling could be
avoided if thermoplastic elastomers would be used
instead of traditional rubbers, as they are completely
recyclable, but the compression set properties of
thermoplastic elastomers (especially at elevated
temperatures) are inferior to those of chemically
vulcanized ones.
6. RECYCLING AND DESIGN
One possible solution (at least in long term) is to
force the manufacturers to collect their products and
to recycle them. This would finally change their
minds not only retrospectively but they would have
to consider recycling from the beginning, which
means that they would have to design their products
taking into account the later recycling technology.
This is a real reverse engineering: disassembly
followed by sorting is much more effective than
shredding followed by sorting [46]. A very good
article is available which summarizes such green
design principles [47], which are listed in Table 2.
Observation of such principles would not solve all
our present problems caused by the traditional design
principles but would diminish the future problems.
Forced application of such, or similar principles
usually meets resistance on the side of the
manufacturers.
They argue that these obstacles reduce
competitiveness and drive away industry. If,
however, such laws are introduced for the whole EU
Table 1 Twelve principles of green engineering from [47]
No. Principle
1:
Designers need to strive to ensure that all
material and energy inputs and outputs are as
inherently nonhazardous as possible.
2:
It is better to prevent waste than to treat or
clean up waste after it is formed.
3:
Separation and purification operations should
be designed to minimize energy consumption
and materials use.
4:
Products, processes, and systems should be
designed to maximize mass, energy, space,
and time efficiency
5:
Products, processes, and systems should be
output pulled rather than input pushed
through the use of energy and materials.
6:
Embedded entropy and complexity must be
viewed as an investment when making
design choices on recycle, reuse, or
beneficial disposition.
7:
Targeted durability, not immortality, should
be a design goal.
8:
Design for unnecessary capacity or capability
(e.g., one size fits all) solutions should be
considered a design flaw.
9:
Material diversity in multicomponent
products should be minimized to promote
disassembly and value retention.
10:
Design of products, processes, and systems
must include integration and
interconnectivity with available energy and
materials flows.
11:
Products, processes, and systems should be
designed for performance in a commercial
afterlife.
12:
Material and energy inputs should be
renewable rather than depleting.

CONTROLLED POLYMER RECYCLING AND DEGRADATION A TUTORIAL 33
(as happened with the REACh legislation in the
chemical industry) we may control the imported
goods as well. At first it does cause additional costs,
but later protects our markets from unfair
competition. It is always a question, who pays the
additional costs? Environmental consciousness is a
luxury for those living at substandard levels.
Purely business-oriented green engineering and
recycling will not work but it has to be considered
that environmental technologies are an asset in the
long run they are necessary. Laws, enforcement and
strict control are necessary but the transition may be
alleviated by temporary state subsidy or selective tax
reduction. Best practices should be promoted if an
ideal solution is not possible.
There are some good examples for the application of
these and similar principles e.g. in a brochure
containing proposals for the packaging industry,
especially for bottle manufacturers [48].
6.1. Pros and cons of controlled
degradation
Another possible (long term) solution for the
recycling problem is if the polymer products are
designed so that they return to the natural carbon
cycle after finishing their useful life. The advantages
of such a concept are obvious:
if the degradation rate is known and controllable,
the lifetime can be designed
the environmental fate of the product is known
the manufacturer will have a competitive edge, a
marketing advantage related to the green
product
new markets or at least niche markets may
become available.
There are, however, not less obvious disadvantages
and risks:
such solutions usually involve expensive additives
or new raw materials
development costs can be enormous, their return
is questionable
the new markets may be risky, slowly developing
and narrow
production should be tightly controlled
decomposition in the planned way requires
precisely observed conditions the consumers
should be educated is disappointment is to be
avoided
the most serious problem is cross-contamination
with traditional plastics, which would render the
recycling of traditional plastics problematic
therefore degradable plastics should be collected
separately (visible identification, labeling)
the planned application should be carefully
designed and engineered to avoid mismatch of
planned an real lifetime
6.2. Controlled photo-oxidative
degradation
There are basically two philosophies used for
controlled degradation: one is based on the controlled
acceleration of thermo-photo-oxidative degradation,
the other is based on bio-degradation. Thermal and
photo-oxidation of most polymers (at least that of
their aliphatic part) is mainly based on a combined
cycle of two cyclic reactions (shown in Figure 10)
which can be controlled by the use of antioxidants
[49].

Figure 10 Basic reactions involved in the thermo-photo-
oxidation of aliphatic polymer chains [46].
Under thermal or light impacts alkyl radicals are
formed which react with the ambient oxygen,
forming peroxy radicals. Peroxy radicals react with
other alkyl chains and hydroperoxides and new alkyl
radicals are formed. Hydroperoxides may undergo
homolysis giving rise to alkoxy and hydroxyl
radicals. Alkoxy radicals may also react with alkanes
and new alkyl radicals are formed. So-called primary
antioxidants (usually sterically hindered phenols or
amines) scavenge the reactive radical species by
forming stable radicals instead, while secondary
antioxidants (usually organic phosphites or sulfides)
deactivate hydroxyl radicals. Certain transition metal
ions may accelerate the left cycle thus leading to
earlier degradation. Such ions are masked by
complexing agents in high voltage polyethylene
insulations where degradation is to be avoided, or
may be added intentionally to agricultural films or
other products, where shortened lifetime is required.

34 Gyrgy Bnhegyi
Pro-oxidants are activated by light or heat under
outdoor conditions. Such (environmentally benign)
transition metal salts are called pro-oxidants and are
available in masterbatch form. Lower molecular
species produced by accelerated oxidation are finally
available for attack by microbes. In some other cases
the degradation does not reach the molecular level,
but very fine polymer powder is formed, which is
neutral and does not endanger the environment. This
process is called oxo-biodegradation [50], its primary
use is in agriculture (mulch films, greenhouse films,
bags for compost collection). In other applications
biological pro-oxidants, as starch, are used which
are more prone to the environmental effects [51].
Companies developing more expensive polymers that
are biologically degradable to the molecular level,
fiercely debate the claim that identification of oxo-
biodegradable films with their products is really
justified [52].
6.3. Biodegradation
In popular green parlance plastics from renewable
resources are frequently mixed up with
biodegradable polymers, but this is a mistake. There
are plastics made of non-renewable resources, which
are not biodegradable these are most synthetic
polymers. There are polymers made of renewable
resources, but non-degradable: an example is
polyethylene made in Brazil from ethanol obtained
from sugar cane. There are polymers, which are
made of synthetic (non-renewable) raw materials, but
are degradable e.g. polylactide can be made from
synthetic lactic acid. And finally there are polymers
made of renewable resources which are degradable
e.g. bacterial polyesters.
When we talk of degradability, it should be clearly
stated under which conditions is the material
degradable (light? heat? humidity? soil? composting?
aerobic? anaerobic?) otherwise the term is
meaningless or misleading. Most frequently used
biodegradable plastics belong to polyesters: e.g. PBS
= polybutylene succinate, PBSA = polybutylene
succinate adipate, PCL =polycaprolactone, PLA =
polylactide or polyesteramides [53]-[55] PLA is in
the most advanced stage as far as applications are
concerned, here the major problems are related to the
price and to the relative rigidity of films, injection
molded or blow molded articles made of this
material. These problems can be alleviated by
copolymerization, plasticization or blending. The
main area of application is food packaging. Proper
composting conditions should always be provided for
the collected biodegradable waste if complete
decomposition is required. At present polymers of
biological origin cannot replace traditional ones in
most applications but a gradual market gain is
expected in the near future.
7. TOWARDS A SUSTAINABLE
PLASTICS TECHNOLOGY
When assessing products and technologies nowadays
Life cycle analysis [56] is performed, which takes a
cradle to grave approach and calculates no only
energy consumption but also CO2 emission, ozone
layer depletion effects, resource consumption,
ecotoxicity and much more. It requires a fairly broad
database regarding raw materials and technologies
and, although the method can be debated especially
the relative weight factors ascribed to the various
effects, this method is presently the most effective
one for assessing the consequences of replacing one
material or technology by another one. Eco-
efficiency assessment of plastics recycling methods
has been performed [57], LCA of a concrete
intractable plastic waste to artificial crude oil
technology [58] is available, a comparative study of
practices in various European countries [59] based on
the LCA philosophy has been issued, and we also
cite a Scandinavian analysis on the economic
background and feasibility of plastics recycling [60].
All these careful studies are necessary to make
concrete decisions, but the simple old saying on the
R-s remains true: reduce, reuse, recycle, recover,
replace!
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