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Mechanical recycling of continuous fiber-reinforced thermoplastic sheets

, ,
Elmar Moritzer and Gilmar Heiderich

Citation: AIP Conference Proceedings 1713, 120013 (2016); doi: 10.1063/1.4942328


View online: http://dx.doi.org/10.1063/1.4942328
View Table of Contents: http://aip.scitation.org/toc/apc/1713/1
Published by the American Institute of Physics
Mechanical Recycling of Continuous Fiber-Reinforced
Thermoplastic Sheets
Elmar Moritzera, Gilmar Heidericha*
a
University of Paderborn, Polymer Engineering Paderborn (KTP), Paderborn, Germany

gilmar.heiderich@ktp.upb.de
elmar.moritzer@ktp.upb.de

Abstract. This contribution examines possible material recycling of offcuts generated during the production of
continuous-fiber-reinforced composite sheets. These sheets consist of a polyamide 6 matrix and glass fiber fabric. In the
initial step, the offcut is shredded to obtain particles; following that, the particles are processed in a twin-screw process to
produce fiber-reinforced plastic pellets with varying fiber contents. These pellets are intended for use in injection
molding processes as a substitution for new raw materials. This investigation centers on the mechanical properties which
can be achieved with the recycled material after both the twin-screw process and injection molding.
Keywords: Composite materials, fiber-reinforced thermoplastics, injection molding, recycling
PACS: 81.05.Qk; 83.50.Uv

INTRODUCTION
In the 21st century, a continually rising demand has been noted for fiber-reinforced plastics with thermoplastic
matrices. The reason for this rising demand are the superior physical and mechanical properties of such composites
as compared to non-reinforced thermoplastics. Fiber-reinforced thermoplastics are predominantly used in injection
molding processes for highly stressed parts; their superior mechanical properties allow them to be used in areas that
have traditionally been the sole domain of metallic materials. Due to the good mechanical strength-to-weight
properties of composites, the total weight of parts can be reduced; additionally, complex part structures can be
economically produced in an injection molding process.
In addition to short-fiber reinforced plastics, continuous-fiber-reinforced composite sheets are increasingly used
in part production. In such processes, sheets are heated to the melting temperature of the matrix polymer and
subsequently re-formed with a tool. With the continuous fibers, mechanical properties can be obtained that are not
possible with shorter fibers. However, freedom of construction is restricted as a consequence of the re-forming
process. By integrating the re-forming process directly into the injection molding process, more freedom of design is
possible. With injection molding functional elements can be created, in addition to the advantages of the
characteristic mechanical properties of continuous-fiber reinforced plastics.
The production of continuous-fiber-reinforced composite sheets is a continuous pressing process. The fibers and
the raw polymer material are fed into a heated double band press; during the process, the polymer melts and
impregnates the fiber fabric. The material is also consolidated due to pressure from the press itself. After leaving the
double band press, the composite is cooled and the continually produced composite band is cut into sheets. This
cutting process necessarily results in the production of offcuts; in addition, later users of the sheets will also produce
offcuts during production of finished products. This large volume of waste material has prompted the search for a
suitable recycling system. The thermoplastic matrix of these materials is advantageous for recycling, as it can be
repeatedly melted and cooled; thus, a material recycling scheme that would utilize offcuts of fiber-reinforced
plastics as the material for an injection molding process is possible.
In order to enable processing on standard injection molding machinery, the material must first be transformed
into a processable state. The material is therefore shredded and subsequently processed in a twin-screw process to
produce plastic pellets or granules. These pellets will later be used as a substitute for new material; for this reason,
their mechanical properties are of particular interest.
The mechanical properties of fiber-polymer composites are primarily determined by the lengths of the fibers. The
fiber lengths found in the material is dependent on the production process used. When processing fiber-reinforced
plastics on screw-based machinery, the process always entails a certain amount of fiber breakage. The mechanisms

Proceedings of PPS-31
AIP Conf. Proc. 1713, 120013-1120013-5; doi: 10.1063/1.4942328
2016 AIP Publishing LLC 978-0-7354-1360-3/$30.00

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leading to fiber breakage can generally be categorized based on the interaction of the fibers with their environment
[1; 2]:
x Fiber/Fiber Interaction: Fiber breakage caused by stress concentration at the point of contact between
the fibers or due to bending loads where fibers overlap. These interactions increase as either the fiber
content and/or the 1/d-ratio increases.
x Interactions between fiber and melt-conveying surface
x Fiber/Polymer Interaction: Fiber breakage caused by the viscous forces transferred via the polymer melt
due to flow speed gradients.

EXPERIMENTAL SETUP
The starting material consists of process-offcuts of continuous-fiber-reinforced composite sheets, which consist
of a polyamide 6 matrix with a 67% glass fiber content. This composite, which consists of an engineering plastic and
continuous fibers, boasts excellent mechanical properties (tensile strength: 400 MPa). The goal is to preserve the
strengthening qualities of the fibers after further processing in an injection molding process. In order to enable use of
the offcuts in such a process, they are firstly shredded in a single-shaft mill and afterwards re-formed to pellets in a
twin-screw process.

Material Shredding
The high-strength fiber-reinforced offcuts require the use of a robust shredding unit. The technology of the
single-shaft mill is particularly suitable for the task, due to its massive, solid construction and its generally high-
powered drive system. For the reduction of the offcuts, a shredder with 18.5 KW drive power and a segment screen
insert with hole diameters of 8 mm and 10 mm is used. With the screen insert the desired particle size during the
shredding process is ensured.
During shredding of the offcuts, the first fiber breakages 50
occur. The fibers are then further shortened during the twin- 45 38.79
screw process. In order to quantify the breakage in the twin-
percentage of particles [%]

40
screw process, the starting fiber length in the shredded 35
material is first measured. This is done with the help of 30
particle size analysis. Under the assumption that there is no 25 21.66
fiber breakage inside of the particles, the size of the particles 20 12.81
13.53 13.21
is taken as an approximation of the fiber length. Furthermore, 15
the sizes of the particles provide the basis to estimate the 10
further processibility of the material in terms of the twin- 5
screw process. In order to ensure that material is able to 0
0-1 1-2.5 2.5-4 4-6.3 6.3-8
effectively enter the screw channel and fill the machine, it particle size range [mm]
must be ensured that the particle size is smaller than the flight FIGURE 1. Particle Size Distribution
depth of the screw in the intake zone.

Pellet Production
The creation of plastic pellets or granules from the shredded material is, in addition to direct processing in the
injection molding process, one of the procedures used in the salvaging of the continuous-fiber composite sheets. The
additional process stage necessary for pellet production causes more damage to the material than direct processing,
where the shredded material is directly fed into the plasticizing unit; this can have a negative influence on the
mechanical properties of the material. The advantage of pellet production is, however, that these pellets can then be
processed on standard injection molding machinery.
To produce fiber-reinforced pellets, the shredded material is fed into a twin-screw extruder with a 25 mm screw
and a ten barrel setup via the main feed. It is additionally possible to feed pure polyamide 6 into the machine via a
side-feed on the barrel. The pellets are created in an underwater process. As the shredded material enters the process
via the main feed, it subjected to a long residence time in the process; the consequent fiber breakage and the
resulting effects on the materials mechanical properties are therefore of particular interest. The material is
processed at a temperature of 270C and at a speed of 350 rpm. The dosing mechanism used during pellet
production uses a Flex-Wall hopper; this prevents blockages in the hopper with cyclical movements of the flexible

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hopper walls. The screw configuration used (FIGURE 2) has been optimized for compounding the shredded material
with pure polyamide.
re-conveying element atmospheric pressure degassing main feeding
conveying element

Mixing element side feeding kneading element


FIGURE 2. Screw Configuration

First, this configuration is used for producing pellets from only the shredded material. In order to reach typical
off-the-shelf fiber content levels (< 50% by mass) in the pellets, an additional step is taken to compound the
shredded material with polyamide 6. In doing so, the shredded material is intended to strengthen the pure polyamide.
By varying the quantity of shredded material added to the polyamide, glass fiber contents of 20%, 30%, and 40% by
mass can be achieved. The material throughputs are mixture-dependent and range from 7 to 12 kg/h.

Production of Test Specimens


In order to determine the mechanical property values of the pellets produced in such a twin-screw process, test
specimens of type 1B have been produced with an injection molding process according to DIN EN ISO 527-2. For
production, an injection molding machine with a screw Diameter of 25 mm and screw with an l/d-ration of 24 is
used. Before producing the test specimens, the pellets were dried for 5 hours at 80 C in a low-humidity air dryer.
As material salvage for such continuous-fiber-reinforced plastics has not yet been examined, a window must be
established within which the material can be processed. This was done by conducting statistically planned
preliminary experiments, in which the influence of such injection-molding parameters as screw speed, processing
temperature, and backpressure were examined to determine their effect on the processing properties. The processing
window of polyamide 6 was used as the basis for these experiments; for production using the pellets, the optimum
process parameters as determined in the preliminary experiments were used.

EXPERIMENTAL INVESTIGATIONS
The test specimens produced in the injection molding process were then subjected to mechanical tests, which
were used to determine the tensile strength, the Youngs modulus, and the impact strength. In addition to examining
the fiber lengths and the fiber content levels in the pellets, the properties of the material were also determined. The
fiber lengths in the pellets can be used, among other things, to determine fiber breakage during the process.
The tensile strength of the test specimens was determined in a single-axis tensile test according to DIN EN ISO
527-1. Using a 10 kN loading cell and an extensometer, stress and strain were measured during the test. Five
specimens per operation point were tested in a freshly molded state.
As a further mechanical characteristic, the impact strength was determined following DIN EN ISO 179-1/1eU.
Five unnotched specimens per operation point were tested in a freshly molded state with a 5 J pendulum
Tensile strength and impact strength are influenced by fiber content and fiber length in the pellets [2; 3; 4], in
addition to other factors; therefore, the fiber length and the fiber content of the pellets was determined. The
measurement of the fiber content was carried out according to DIN EN ISO 3451-1. The matrix polymer was ashed
in an oven at 600 C and the remaining fibers were gravimetrically analyzed. The mass of the fibers was related to
the starting mass of the specimen in order to determine the fiber content . The measurement of fiber length was
conducted as an optical measurement of the fiber residue. The fibers were separated in a carrier fluid, placed on a
microscope slide, and digitalized with a scanner. A graphic analysis software then allowed the fiber lengths to be
determined.

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RESULTS
The mechanical properties achievable with the pellets can be seen in the evaluation of the results from the tensile
and the impact tests. In FIGURE 3, the tensile strength, the Youngs Modulus, and the toughness are shown for the
compounded material (GF 20, GF 30, GF 40), for the pellets made purely from recycled shreds (GF 60), and for the
polyamide 6 used for the compounding (B30S). For purposes of comparison, another conventional polyamid 6
material (BKV 60) with a glassfiber content of 60% was examined. Its material characteristics are similar to the
pellets produced purely from recycled material.
tensile strength impact strength
250 140 25000
218.18 21536

young's modulus [MPa]


120 20171

impact strength [kJ/m]


tensile strength [MPa]

200 178.91 20000


100
150 80 15000
115.93
95.22 60 8520
100 78.60 10000
40 6453
43.18 5137
50 5000 2696
20
0 0 0
B30S GF 20 GF 30 GF 40 GF 60 BKV 60 B30S GF 20 GF 30 GF 40 GF 60 BKV 60

FIGURE 3. Mechanical Properties

FIGURE 3 clearly shows that the addition of recycled material to pure polyamide results in increases in the
tensile strength and the Youngs modulus. For the impact strength, however, the addition of recycled material does
not lead to any noticeable improvement. The mechanical properties of the pure recycled material are significantly
higher than those of the compounded materials; this can be linked to the high fiber content (64%) of this material. A
comparison with commercially available pellets (BKV 60) shows, however, that there is still considerable room for
improvement in the properties of the recycled material. In addition to the 46 kJ/m higher toughness, the tensile
strength of the commercially available material is about 40 MPa higher than that of the recycled material. Only the
Youngs modulus shows no significant difference.
Aside from the mechanical properties, the fiber content and fiber length in the pellets was determined. As the
fibers are the primary load-bearing elements in the composite, the fiber content and length are crucial characteristics
that provide information about the mechanical properties of the composite material [4]. First, the measurements of
the fiber content show that the pellets produced with the addition of polyamide contain the demanded fiber contents
(TABLE 1). Furthermore, it can be seen that roughly similar average fiber lengths are obtained during the process.
One exception is the pellets with a fiber content of 20% by mass; here, a higher incidence of fiber breakage occurs
due to the high flow of added solids via the side feed. A look at the commercially available pellets reveals a notably
higher average fiber length; this explains its superior mechanical qualities in comparison to the recycled material.

TABLE (1). Material Properties


GF 20 GF30 GF 40 GF 60 BKV 60
Mittlere Faserlnge [m] 249,56 260,51 259,74 253,24 303,72
Gemessener Faseranteil [Ma.-%] 20,38 29,47 38,93 63,67 61,75

SUMMARY AND FUTURE PROSPECTS


In this paper, a procedure is examined for the recycling of offcuts resulting from the production of continuous-
fiber-reinforced composite sheets. This process is intended to enable the resulting offcuts, which consist of
polyamide 6 with a 64% glass fiber content, to be further processed in order to produce fiber-reinforced plastic parts
via injection molding. To do so, the material is first shredded and subsequently used to produce pellets for further
use in a twin-screw process; these pellets are produced both purely from recycled material, as well as with the

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addition of polyamide 6. The mechanical properties of the pellets produced were the focal point of the investigations
described here. The tensile strength, the toughness, and the Youngs Modulus were determined in the course of the
investigations; from these investigations, it is clear that the recycled material offers lower tensile strength and
toughness than comparable new, commercially produced material; the stiffnesses are, however, comparable. The
reason for the inferior mechanical properties is the shorter fiber length in the pellets, which is a result of multiple
process stages and resulting increased levels of fiber breakage.
Further experiments are planned to examine possibilities of process optimization which will allow for the
production of recycled material in twin-screw processes with average fiber length comparable to that of
commercially produced new material. Firstly, a reduction in the residence time of the fibers by using a side feed for
the recycled material will be realised. With different side feed position the influence of the residence time on the
fiber length will be investigated. In addition, influences from machine parameters, such as the barrel temperature
and the screw speed, will also be examined in terms of their influence on fiber breakage.

ACKNOWLEDGMENTS
This work is financed with funds of the European Union and the state North Rhine-Westphalia as part of the
competition CheK.NRW (funding reference number: 31 01 047 02). A special thanks to Bond Laminates GmbH for
providing the material that was used in this investigation.

REFERENCES
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(1983) 13.
2. A. Radtke, Steifigkeitsberechnung von diskontinuierlich faserverstrkten Thermoplasten auf der Basis von
Faserorientierungs- und Faserlngenverteilungen, Ph.D. Thesis, Universitt Stuttgart, 2008
3. M. Metten, M. Cremer, Langfaserverstrkte Thermoplaste spritzgieen in Kunststoffe 90 , Mnchen: Carl Hanser Verlag,
2000
4. G. W. Ehrenstein: Faserverbundkuststoffe, Mnchen: Carl Hanser Verlag, 2006

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