End of Life Solutions for Metallised Polypropylene: A

A Study on Thermal & Mechanical Properties

ABSTRACT

The weight of multilayer packaging film generated annually is about 16 million and the recent
developments that the world has seen in terms of recycling suggests that this kind of packaging
waste should also be reclaimed.

This paper discusses the method to recycle the metallised packaging films which comprised a
plastic layer including polypropylene (PP) and Polyethylene (PE) as main components and an
aluminium layer.

Nowadays, the melt blending of two or more polymers is proved to be an easy and effective
way to give rise to new polymeric material with novel and targeted properties at a relatively
low cost compared to developing entirely new polymeric material.

The present work shows a process for converting metallised packaging waste in the form
Polypropylene or used Metallised PP as a starting raw material to various utility products.

Particularly the material developed has been used to manufacture mobile charger casing.

Post industrial waste of metallized polypropylene is been collected from Uflex and run through
EREMA machine which first convert the waste it to small flakes and then the compacter helps
to further reduce the size of flakes to finally form semi solid. The compounds prepared have
been evaluated for mechanical properties and thermal properties also discussed in this paper.
Tests such TGA, DSC, Flexural and Tensile have been performed to have an idea about the
thermal and structural properties of the recycled material.

INTRODUCTION also been use for decorative applications.

Metalized PP films generally used gives
optimal solution in terms of high oxygen,
gas barrier levels, aroma and flavour
retention. It also helps in significantly
improving water vapour barrier level.
Metalized PP films in past showed its
usefulness through its special optical
properties and a metallic look which has
Although market of metallised PP films is
growing continuously there are no
established sustainable ways to recover and
recycle post-consumer and post-industrial
metalized PP films waste and we have not
discovered any applications of this material
which is present in thousands of tonnes in
our environment. While PP/PET recycling
industries has doing its job for several
decades and proved as the most acceptable
material recycling, metalized PP films are
discarded as waste which mostly ends up in
the landfills. As today’s consumer has
grown up and is more aware towards plastic
recycling, it demands creativity in recycling
of metalized PP films and its subsequent
applications. There are no known
commercially existent metalized PP films
recycling facilities in the world.
Thus, alarming rate of depletion of these
resources gives rise to demand of generating
alternative ways to reduce the consumption,
reuse and recover the material as much as
possible.
The aim of our work is to develop the
material from these metallised packaging
which is at present time is nothing but a
form of waste once it is used for its intended
use.
Also in order to increase the life cycle of
these material and reduce the carbon
footprint, metalized PP films needs to be
recycled effectively and its suitable
application should be chose so that it can
incur substantial value to the product
formed.
MATERIALS
The following material was used for the
present study.
H110MA,from Reliance industries Ltd
India.
Apart from this the material used for study
was Post Industrial laminates which
comprises of Biaxially Oriented
Polypropylene (BOPP), Aluminium and
layers of Polyethylene.
Toluene is used for the experiment of
solvent casting.
METHODS
1. (Material Development)
The objective of our work is to use
metallised PP waste in to some utility
products of daily life.
Also our aim was to utilise the metal Al in
the developed material as filler and
reinforcing agent and that’s why we did not
bothered to separate Aluminium from
Polypropylene.
Also we knew that after Recycling the
properties of film will not be the same and it
may degrade up to some strength keeping
this in mind we have opt for open loop
recycling as making films again would be of
low value.
Through literature review its been concluded
that mechanical recycling should be
preferred over chemical recycling and
incineration practice, and it would be best
option to consider for our material as it will
open the doors for manufacturing of variety
of products as per properties and required
applications.
The cutter compactor technology is used in
our research work that connects to a
continuously filled extruder which pelletized
the post industrial waste that is being
feeded. The washed or unwashed metalized
PP films are fed into the cutter-compactor
where the material goes through several
steps, cutting, mixing, heating, drying (to
remove moisture and prevent the
undesirable hydrolytic degradation)
densification and buffering. Densification
process can also be achieved using an
agglomerator which also have the same
function of compacting and further
improving bulk density of the material.
Then, dried and compacted metalized PP
film is fed into the plasticating extruder
where devolatilization and homogeneous
mixing takes place. The PP melt is then
cleaned in the self-cleaning filter. Following
this, the melt is conveyed pelletizer to obtain
uniform and consistent recycled PP pellets.
Extrusion process is the step where various
additives can be added to enhance the
properties of the PP pellets. This could be
change of colour or chain extenders or any
other functional additives. Here green colour
was added to the waste metalized PP films
during the extrusion process to achieve
green colour recycled PP pellets.
The process of Melt compounding can be
explained stepwise.
(i) Collection of waste or used metalized PP
film which can be Post Industrial as well as
Post-consumer waste.
(ii) To obtain crushed film or flakes by
reducing the size of waste or used metalized
PP film either before or after washing by
cutter-compactor;
(iii) Densifying the film or flakes obtained
earlier in a agglomerator to increase the bulk
density of the film or flakes
(iv) Feeding of the obtained material from
compactor into an extruder for
devolatilizing, homogenizing and converting
the material into melt;
(v) Conveying the melt into a pelletizer to
obtain recycled PP pellets which can use for
different purpose.
All these process has been performed in a
single machine i.e Erema' TE.
SAMPLE PREPARATION
The granules derived from the melt
compounding have been used to make
samples.
We have divided our samples in to five
categories based on different formulation of
recycled metallised film content and amount
of virgin Polypropylene content in it. It
should be noted that virgin refers to
H11OMA grade polypropylene.
The five different formulations are:
(i) 100 % recycled metallised film
(ii) 75% recycled metallised film +
25% virgin Polypropylene
(H110MA)
(iii) 50 % recycled metallised film +
50 % virgin Polypropylene
(H110MA)
(iv) 25 % + recycled metallised film
+ 75 % virgin Polypropylene
(H110MA)
(v) Virgin Polypropylene (H110MA)
INJECTION MOULDING
This injection moulding is used to prepare
samples of different shapes as per
requirements.
Specimens for flexural test
Different specimens are prepared based on
the requirement of test methods used.
Various moulds as per standards are used
while preparing specimens. Mould
temperature, pressure, extruder screw RPM
were important parameters.
The mechanical properties like Tensile
Strength, Flexural Strength and other
physical properties has been calculated to
demonstrate that the material developed can
be used for suitable applications.
EXPERIMENTS
 Mechanical Tests
1. Tensile Testing
The test was performed according to ISO
527-2-1A and it is repeated for 8 samples.
The values so obtained from the tensile test
are comparable to virgin polypropylene
(H 110MA) and hence we can say that the
recycled metallised film material is good to
put use where tensile strength is concerned.
Here we can see that tensile strength is
maximum for virgin and PP and second best
is for recycled metallised film. Apart from
this modulus maximum load capacity and
extension at maximum load also shows
relatively good values and assure that it will
be a good option to consider this material
when tensile strength is concerned.
 For the Metallised film recyclate as the
percentage variation increasing the flexural
strength is decreasing. Except for 50 % , that
too variation is not much significant. So it can
be concluded we are able to retain the flexural
properties of recycled metallised film.

2. Percentage Elongation
Composition of Metallised % Elongation in sample
films Recyclate specimen
0 276
25 271
50 278.43
75 341
100 280
The percentage elongation is increased due
to increase in metallised content and it is
evident from the Young’s modulus itself.

Young’s modulus is increasing and so as the

percentage elongation

3. Flexural Testing
Flexural test is a kind of mechanical testing
in which a concentrated force is required to
bend a cantilever beam under three point
loading system. Flexural test provide us As we can see for the recycled Metallised film,
modulus which is an indication of a material’s as the percentage variation increasing the
stiffness when flexed. flexural strength is decreasing.

The test was performed according to ISO 178 This can be understood by phase
standard for testing of our specimen with morphology of the material.
dimensions (4 x 10x 80) mm by the strain rate
of 1.36 mm per minute. Flexural Strength VS Recyclate %

46
FLEXURAL STRENGTH

44
42
40
38
36
34
0 25 50 75 100
RECYCLED METALLISED FILM
As aluminium content is increasing in
the matrix it creates slight hindrance
in the bending as material is tending
towards brittleness.
Al % from SEM images
6 5.21
4 3.11

Al %
1.52
2
4. Field Emission Scanning 0.196
0
Electron Microscopy) 0 25 50 75 100 125
% recycled metallised PP
Dispersion of Aluminium Particles in the
Polypropylene Polymer Matrix
SEM images shows that the distribution of
aluminium is not uniform or homogenous
throughout the matrix of PP. At some places
they are agglomerated and are distant at
others .

With the introduction of recycled metallised

PP the roughness of the surface is increased.

With increase in percentage of recycled

metallised PP in the blend we see more
Aluminium particles in a given area.

The shape and size of Aluminium particles

The shining particles in the above picture
is not same, it is very irregular.
represents presence of Al particles.
6. Weight by volume ratios
5. Percentage of Aluminium (Density)
Densities of different formulation are
content obtained by dividing the weight of the
samples by their volume.
(Surface area of Al / Total
Material Weight by
image area) *100 formulation Volume ratio

%Metallisation 25 50 75 100 Virgin PP 0.9023

25 % M 0.9218
A/A% of Al 0.196 1.52 3.11 5.21 50% 0.9094
75 % 0.9097
100 % 0.9205
 RECYCLED METALLISED FILM VS MFI
7. MFI ( Melt flow Index )
Percentage of recycled MFI Value
BOPP (Bi-axially Oriented Polypropylene) metallised film
is used for manufacturing of metallised film gram/10 min
with ranges from 3 to 5. 100 8.4

In the present work, the overall MFI which 75 13.12

we are getting for 100 % Recyclate 50 13.46
metallised film is 8.4 (gram/10 min/2.16 25 15.42
kg/230 degree Celsius)
0 (Virgin PP) 36.23
As the weight percentage of the LDPE is not
much as comparison to BOPP so we can say Here from the above values of MFI we are
that it has insignificant effect on increasing getting a decreasing graph of MFI as the
the MFI of recycled polymer. recycled metallised content is increasing.

Whereas it can be estimated that due to RECYCLED METALLISED FILM VS MFI

aluminium MFI is increased significantl as

the percentage of aluminium (Surface Area
of Al / Total Area) % is low i.e 5.21 % it
could not increase up to that extent where it
can be comparable to virgin PP which has
far higher value.

The standard used for measuring MFI is

ASTM D1238
(gram/10 min/2.16 kg/230 degree Celsius) For Virgin PP the MFI is of highest vlue and
for recycled metallised film it is least as can
be seen from bar chart.

RECYCLED METALLISED FILM VS MFI

Thermal Properties Degradation temperature
252.065 256.051
1. TGA (Thermo gravimetric 280 236.09 231.22 227.2
analysis) 240
200

Temp
TGA measures the rate (velocity) and 160
120
amount of deviation in the mass of a sample
80
as a function of temperature or time in a 40
controlled atmosphere. The estimations are 0
utilized essentially to decide the thermal 0 25 50 75 100 125
% of recycled metallised film in blend
and/or oxidative qualities of materials and
also their compositional properties.
in the blends, thermal stability decreases
and it starts degrading earlier. It is due to
shortening of polymeric chains i.e chain
scission.
It is also to be noted that the temperature
shown below is the initial temperature where
degradation has just started. However the
extreme degradation can be shown in
different graph of DTG Curves

2. Derivative Thermo gravimetric

Analysis (DTG)
Instrument name: NETZSCH TG 209 F3
It is obtained from TGA analysis and
Type of crucible: Al2O3
provides information about the temperature
Atmosphere: Nitrogen
at which the degradation rate is maximum
Range: 30 to 850 deg C
and also in how many stage the degradation
Rate of heating: 10 deg / minute
has taken place. It is a very important
From TGA we have found that degradation parameter for processing any polymer at
temperature is reducing from virgin PP to
100% recycled metallised PP. high temperature.

However, only 75% recycled metallised film
sample readings are showing anomalous
behaviour.
It can be concluded from these graphs that
with increase in % of recycled metallised PP
Different DTG curves shown below helps to
understand the behaviour of material,
recycled as well as Virgin PP.
Table shows data for all formulations.
 DTG curve for Virgin PP 3. DSC (Differential Scanning
2.00E+00
Calorimetric)
DTG
0.00E+00
0 200 400 600 800 1000 This technique is used to study effects of
-2.00E+00
heating on polymers and obtaining values
-4.00E+00
of melting point.
-6.00E+00

-8.00E+00
Instrument name: NETZSCH DSC 200 F3

-1.00E+01 Reference: Polypropylene

-1.20E+01
Atmosphere: Nitrogen

DTG curve for recycled metallised film Temperature range: 30 to 250 deg C

2.00E+00 Heating rate: 10 Deg C/minute

0.00E+00
DTG
-2.00E+00 0 200 400 600 800 Below graphs represent the curves obtained
-4.00E+00 through DSC test and the downward peaks
-6.00E+00
symbolises the melting point of the material.
-8.00E+00
-1.00E+01
-1.20E+01

Complete degradation for 100 % recycled

metallised film

Degradation with temp

150
2.Recycled metallised polypropylene
100
Mass%

50

0
0 200 400 600 800
Temp(deg C)

The above graph show mass percentage

variation as the temperature increases.
Melting point of all the formulations is
shown in table as obtained from these
graphs.
RESULTS & DISCUSSIONS
Influence of Metallisation on Mechanical
properties due to recycling
Tensile
Metallisation or aluminium in the material
content have little or no effect in decreasing
tensile properties. It can be stated in other
way as the percentage of Aluminium (Area
/Area % ) is very less between 0 to 5%,
which is considered to be significantly to
alter the properties up to much extent.
Similarly change in modulus is also
insignificant. Percentage increase in
Young’s Modulus is 1.77 obtained for the 50
% M.
Flexural
It is been observed that the flexural values
obtained have relatively equal values and
changes is insignificant.
The maximum change or reduction is found
to be 11% for 25 % recycled metallised film.
However it is also clear that increase in the
metallised percentage has detrimental effect
on flexural strength, as the metallised
percentage film recyclate varies from 0 to
100%.
So it can be concluded that metallisation or
aluminium content has negative influencing
on the flexural properties up to some extent
especially on flexural strength.
Melting point
We found that melting point decreases with
increasing % of recycled metallised PP in
the blend (from 165.976 for virgin PP to
163.968 for 100% recycled metallised PP).
But the change is very little i.e. around 2
Deg C therefore we can say that presence of
Aluminium particles does not much affect
the melting point of the blend.
Only one endothermic melting peak for the
blend shows that the virgin PP and recycled
metallised PP are miscible with each other.
After the successful study it also has been
observed that percentage elongation is
increased due to increase in metallised
content and it is also evident from the tensile
modulus itself.
By, TGA analysis it is being referred that
starting temperature of degradation
decreases sharply from virgin PP to 100%,
the values are 236.09, 231.22 and 227.2 Deg
C for 25%, 50% and 100% recycled
metallised PP, but it is very close to each
other.

The minimum degradation temperature in all

the five composites is 227 Deg C, therefore
the injection moulding temperature 220 Deg
C used for making these samples is safe.
To demonstrate the usefulness of our
CONCLUSION developed material. This recycled material is
used in manufacturing of Charger casing and
To encounter the recycling challenges and
the same is shown below.
keeping environment safety into
consideration the present research work comes
out with a process for converting used/waste
metalized PP films into recycled PP as a
starting raw material for various utility
products. Hence, an environmental friendly
process for recycling of metalized PP film is
developed to produce recycled PP pellets with
comparable physical, mechanical, optical and SUMMARY OF RESEARCH
aesthetic properties.
This paper discusses the technique to create
There are number of applications of this value out of waste which is present in ample
material which is developed by waste amount in our environment. Though this
metallised PP film and the utility of this paper helps researchers to carry out further
material is confirmed through all the studies and finds out suitable applications
mentioned test for different properties. depend upon the material properties
Building insulation board, Roof Tops obtained through mechanical and thermal
characterisations.
Gas cylinder stand
Also the data obtained is for Post industrial
DVD and CD cases waste and few additional steps like washing
& drying should be taken in order to get
Garden furniture and fencing
better properties.
 Garden sheds and composters
The most important aspect of Recycling of
 Seed trays, flower pots metallised polypropylene which exist in
 Office accessories and partitions waste as films is to collect sort and get
ready for the processing.
To be having continuous supply of this
waste as raw material is a great challenge for
recycling industries who are willing to work
in the recycling of metallised PP.

Most of the time recycled products are

considered to be a low value products and
this idea has given wrong insight in the mind
of consumers.

Also, the cost of collecting, processing and

converting in to products exceeds the
overcall cost of product if it is made out of
virgin material and that further provides
hindrance to utilisation of recycled material.

We need to find appropriate applications of

this material where it can materials of
equivalent value.

The government should give subsidies to the

industries who are working in the recycling
fields so as to empower these industries who
are working for cause and helps in saving
the environment.

With the support of government, public

awareness, researcher’s effort in this field to
find suitable and potential application we
will be able to commercialise the use of this
metallised Packaging PP waste in to
products very soon.