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a
Politecnico di Milano, Dipartimento di Meccanica, Via La Masa 34, I-20156 Milan, Italy
b
Radici Plastics, Chignolo d’Isola BG, Italy
Received 8 June 2006; received in revised form 28 September 2006; accepted 30 September 2006
Abstract
The mechanical recycling of short fibre reinforced thermoplastics by granulation and subsequent injection moulding allows for recov-
ery of both post consumer waste and in-plant recycled material in many industrial sectors. Parts made of these materials are often sub-
jected to cyclic loads and therefore need to be designed against fatigue. The fatigue behaviour of reprocessed glass fibre reinforced
polyamide 6,6 has been studied, using standard injection moulded specimens containing different percentages of recycled material.
The effect of reprocessing of clean materials is mainly represented by fibre shortening in the injection moulding process and consequent
degradation of the load bearing capacity of material. The relationship between the fatigue strength and the fibre length distribution has
been discussed.
2006 Elsevier Ltd. All rights reserved.
Keywords: A. Recycling; Short glass fibre reinforced thermoplastics; B. Fatigue; E. Injection moulding
1359-835X/$ - see front matter 2006 Elsevier Ltd. All rights reserved.
doi:10.1016/j.compositesa.2006.09.012
A. Bernasconi et al. / Composites: Part A 38 (2007) 710–718 711
between the glass fibres and the polymer are affected by the the fatigue strength of SGFR polyamides is particularly
injection moulding process. Bonding can be improved by relevant for the increasing number of load bearing applica-
using coupling agents or by incorporating recycled material tions subjected to repeated loads. For this reason, and for
into virgin material, but fibre shortening constitutes an the increasing industrial interest about recycled composite
important issue for safely using recycled fibre reinforced polymeric materials, we investigated on the effect of repro-
materials. With chemical recycling the fibres and the poly- cessing (in-plant recycling) on the fatigue strength of a
mer are recovered and reused separately. Separation gener- short fibreglass reinforced polyamide.
ally consists of dissolution of the matrix and separation of
fibres. Apart from costs, this may cause safety and environ- 2. Experimental
mental concern, due to the handling and use of the large
amount of solvents required. However, condensation poly- 2.1. Materials and processing
mers such as PET and polyamide can also be de-polymer-
ised, i.e., returned back to their original constituents, by Extrusion compounded pellets of a short glass fibre rein-
hydrolysis. The polymerisation process is reverted and forced polyamide 6,6 containing 35% by weight of fibres
the material broken down to initial monomers. Fibres (PA66 GF 35) were injection moulded into tensile test spec-
can be separated and the monomers used to produce new imens using a Sandretto Serie 7 HP 95 T injection mould-
composites with addiction of new reinforcements. ing machine with maximum injection capacity of 160 cm3/s
Among the different types of polymers, we concentrated and a screw diameter of 45 mm. Injection moulding vari-
on short glass fibre reinforced (SGFR) polyamides, which ables are reported in Table 1.
are widely employed by the automotive industry, for parts The in-plant recycling of the virgin material consisted of
located in the engine compartment and also for load bear- grinding of tensile test specimens in a Dipre GRS 182 A7
ing applications, like the clutch pedal of several car models. granulator of 2.2 kW power at 300 rpm, equipped with 7
Fibreglass reinforced polyamides can be easily recycled by rotary blades and 1 stationary blade of 75 mm length
granulation and remoulding. This process is also of par- mounted on a 180 mm diameter rotor, and subsequent
ticular interest for users of virgin materials, because the injection moulding of specimens containing a blend of vir-
so-called in-plant recycling of off-specification parts and gin and recycled material. A total of four batches of spec-
production scraps is commonly performed. In this context, imens were manufactured, with a content of 0%, 25%, 50%
the mechanical behaviour of reprocessed fibreglass rein- and 100% of reprocessed material. The corresponding val-
forced polyamides has been studied by Eriksson et al. [3], ues of the regrind level, defined as the ratio of the mass of
by submitting injection moulded specimens containing dif- the reprocessed material and the total mass of the speci-
ferent percentages of in-plant recycled material to tensile men, i.e.,
and impact tests. The results of these experiments showed M recyclate M virgin
that the degradation of the composite is mainly related to RL ¼ ¼1 ð1Þ
M tot M tot
the fibre shortening occurring during successive injections,
whereas reprocessing has little if any effect on the proper- ranged from 0 (virgin material) to 1 (material containing
ties of the matrix and of the fibre–matrix interface. 100% of reprocessed material).
On the other hand, unlike in-plant recycled materials,
the mechanical properties of recycled materials originating 2.2. Mechanical testing
from post consumer waste are influenced by factors affect-
ing the matrix properties and the fibre–matrix interface, Mechanical testing consisted of tensile and fatigue tests.
like the presence of impurities and the effects of service, Tensile properties were measured in accordance with the
which implies ageing (thermal oxidation) and fluid contam- procedure in ISO 527-1 standard [11] at crosshead speed
ination. An experimental investigation on these effects on a of 5 mm/min on an MTS Alliance RF 150 machine. Strains
fibreglass reinforced polyamide (both virgin and repro- were measured with a MTS 634.25 extensometer of 50 mm
cessed) has been performed by Eriksson et al. [4], by testing base length. Specimens for both tensile and fatigue tests
samples containing glass beads in order to simulate the had size and dimensions of type 1A tensile test bars,
presence of impurities, and by submitting specimens of according to ISO 527-2 standard for tensile tests [12].
the same material to tensile and creep tests after controlled
thermal and coolant ageing [5–7]. The experimental values Table 1
Injection moulding variables
of the tensile and impact tests of in-plant recycled SGFR
polyamides were predicted by Eriksson et al. [8] on the Mould temperature 70 C
Barrel temperature 270–275 C
basis of the fibre length distributions, by applying a method
Melt temperature 280 C
originally proposed by Bowyer and Bader [9], using a mod- Injection time 3.5 s
ification of the Kelly–Tyson model [10]. Cooling time 6s
These studies concentrated on tensile strength, impact Total cycle time 18 s
resistance and creep of reprocessed SGFR polyamides, Back pressure 5 bar
Hold pressure 60 bar
whereas no fatigue test results were reported. Actually,
712 A. Bernasconi et al. / Composites: Part A 38 (2007) 710–718
Table 3
Results of the tensile tests for the different blends of virgin and reprocessed PA66 GF 35
Material Elastic modulus (GPa) Tensile strength (MPa) Stress at break (MPa) Strain at break (%)
Virgin 10.84 (±0.14) 187.9 (±2.4) 187.4 (±2.7) 2.87 (±0.13)
25% reground 10.75 (±0.13) 185.9 (±0.5) 185.3 (±0.6) 2.85 (±0.06)
50% reground 10.73 (±0.09) 181.6 (±0.7) 180.5 (±1.2) 3.00 (±0.06)
100% reground 10.27 (±0.12) 167.3 (±1.6) 165.5 (±1.4) 3.04 (±0.09)
Table 4
Values of the fatigue strength coefficient and exponent of the PA66 GF 35 samples containing different percentages of reground material
Material rf (MPa) b [–] rw (N = 105) (MPa) rw (N = 106) (MPa)
Virgin 240.5 0.0666 111.7 95.8
25% reground 242.7 0.0686 110.2 94.1
50% reground 219.4 0.0623 107.1 92.8
100% reground 213.6 0.0683 97.3 83.1
stress, in spite of the small differences between the values of mechanical parameters with FLD and provides the follow-
the fatigue strength coefficient, there is a factor of 10 ing expression for the tensile strength of a SGFR
between the numbers of cycles to failure of virgin material composite
and that of the 100% reprocessed composite. ( )
lX lj ¼1
i ¼Lc
sli vi X Lc
rM ¼ g 0 þ ruf vj 1
li ¼0
d lj ¼Lc
2lj
4. Discussion
þ ð1 vf Þr0m ; ð5Þ
4.1. Relationship between FLD and composite strength
where d is the fibre diameter, s the interfacial shear
Elastic modulus and ultimate tensile strength are plotted strength, li the length of fibres whose volume fraction is
in Fig. 5 vs. the weight average fibre length, together with vi, ruf is the tensile stress of fibres, r0m is the stress carried
the corresponding values of the regrind level (values of by the matrix at the fibre failure strain, Lc is the fibre crit-
Lw,adj are decreasing for increasing RL). Thus, it seems rea- ical length and g0 is an orientation factor. Subscripts i and j
sonable that fibre shortening is responsible for the varia- refers to fibres of sub-critical and super-critical length,
tion of the tensile properties, in agreement with the respectively. The expression for the critical length is
results presented in the cited references. Lc = rufd/2s.
Further understanding of the relationship between FLD The micromechanical parameters ruf, s and g0 can be
and composites strength can be provided by micromechan- identified by applying an iterative method proposed by
ical models, like the Bowyer–Bader model, based on a Thomason [15–17] for materials with non-linear stress
modified Kelly–Tyson model, which combines some micro- strain relationships. The method consists of extending the
A. Bernasconi et al. / Composites: Part A 38 (2007) 710–718 715
validity of Eq. (5) to describe the full stress–strain curve of the additional thermal cycles corresponding to subsequent
a composite prior to failure, obtaining the relationship injection mouldings.
( lj ¼1 ) Even with these limitations, the model allows predicting
lX
i ¼Le
sli vi X E f ec d with high accuracy the reduction of strength for a 100%
rc ¼ g0 þ E f e c vj 1
li ¼0
d lj ¼Le
4slj content of reprocessed material, whereas the reduction
observed in samples containing 25% and 50% of reground
þ ð1 vf Þrm ; ð6Þ specimens is lower than predicted values. Thus the sensitiv-
where rm is the stress carried by the matrix at the ity of the model to small variations of the FLD seems to be
composite strain ec, and the critical length is replaced by higher than that of the material itself. Moreover, predic-
Le = ecEfd/2s. Thus, values of s and g0 can be determined tions could be improved if models for the variation of the
by making prediction provided by Eq. (6) coincide with micro-mechanical parameters with reprocessing were avail-
experimental stresses recorded in tensile tests for a mini- able. However, predictions are on the conservative side.
mum of two strain level; finally, the value of ruf is obtained By observing the dependence of the fatigue strength at
by equalling the composite tensile strength to the predic- 106 cycles to failure upon the average fibre length, as shown
tion obtained by applying Eq. (5). in Fig. 6, one may suppose that a similar relationship
A comparison between experimental and predicted val- between FLD and fatigue strength exists as well. This is
ues of the ultimate tensile strength of the four blends of further confirmed by the normalised S–N curves of
PA66 GF 35 is reported in Table 5. Composite strength Fig. 7, obtained by dividing maximum stress values by
values were predicted by applying the method proposed the tensile strength of the material sample under examina-
by Thomason, with s = 45 MPa, g0 = 0.67, Lc = 200 lm. tion. All the experimental data fall within the 10–90% pre-
The value of these parameters were determined with tests diction band of the S–N master curve. This signifies that
on the virgin material and subsequently employed to pre- the fatigue strength is proportional to the tensile strength.
dict the strength of the samples containing reground mate- This is a general relationship valid for most of the short
rial, applying Eq. (5) to their respective FLDs. Values of fibre reinforced thermoplastics, provided that fatigue tests
rm were obtained from tensile tests on samples of unrein- are always run using the same specimen geometry, at the
forced PA66 matrix. same frequency and tensile tests are conducted at the same
The values of s, Lc and g0 parameters were kept con- strain rate.
stants for all materials in order to test the ability of the It can then be concluded that, for the particular case of
model to predict the tensile strength values of material materials having the same composition but different FLD,
samples containing reprocessed material on the basis of the modified Kelly–Tyson model is applicable to the pre-
their FLDs and the properties of the virgin material. Actu- diction of the fatigue strength as well, provided that the
ally, a variation of these parameters with the content of values of the fatigue strength coefficient and the exponent
reprocessed material may be expected. In fact, the g0 are known for the virgin material. In fact, on the basis of
parameter is related to the fibre orientation distribution, the FLD of the reprocessed material, which can be easily
which is affected, among other factors related to the injec- obtained with relatively simple analysis tools, and the
tion moulding process, by the fibre properties, particularly micromechanical parameters derived from tensile tests on
the FLD. The variation of g0 for a reprocessed 30% fibre- the virgin material, the ultimate tensile properties of the
glass reinforced polyamide 6,6 was supposed to be negligi- reprocessed material can be predicted. Then, these data
ble by Eriksson et al. [3], who supported this assumption by
comparing the variation of stiffness as a function of the
angle to the flow direction of injection moulded specimens
of virgin and reprocessed material. However, no direct
measurement of the fibre orientation distribution was
available for the specimens used in this work. Moreover,
reprocessing is likely to modify the interfacial shear
strength, and consequently the critical length, because of
Table 5
Values of the tensile strength of the PA66 GF 35 samples containing
different percentages of reground material as predicted by the modified
Kelly–Tyson model, compared to experimental data
Material rM Bowyer–Bader rM Experimental Error
(MPa) (MPa) (%)
Virgin 188 188 –
25% reground 175 186 5.9
50% reground 169 182 7.1
Fig. 6. Fatigue strength at 106 cycles to failure of the PA66 GF 35 as a
100% reground 165 167 1.2
function of the weight average fibre length.
716 A. Bernasconi et al. / Composites: Part A 38 (2007) 710–718
Table 6
Comparison of the tensile properties of virgin PA66 GF 35 DAM and
conditioned
Material E (GPa) rM (MPa) eb (%)
DAM 10.84 (±0.14) 187.9 (±2.4) 2.87 (±0.13)
Fig. 8. Comparison of the S–N curves of PA66 GF 35 in the DAM and
Conditioned 7.71 (±0.11) 125.8 (±0.1) 5.11 (±0.32)
conditioned state.
A. Bernasconi et al. / Composites: Part A 38 (2007) 710–718 717
bridged by highly deformed matrix filaments until final Tests were run with specimens in the dry as moulded
fracture occurs), whereas the same material in the DAM state. The effect of water content has also been investigated
state shows a more brittle behaviour at the microscale. on the virgin material only, in order to provide a quantita-
The effects of moisture absorption are also important for tive assessment of the modifications of the S–N curves tak-
the design against fatigue of real parts, which are prone to ing place when the material is conditioned, i.e., has been
water absorption. Therefore, care must be exercised when allowed to absorb water. Ductility of the matrix is
using the master S–N curve of Fig. 7, obtained with DAM enhanced by the presence of water and therefore mechani-
specimens, to design parts against fatigue, in order not to cal properties are modified. Stiffness, tensile strength and
neglect the reduction of strength and the change in slope. fatigue strength are considerably lower than those of the
In facts, the fatigue assessment of parts containing repro- DAM material, whereas the elongation at break is higher.
cessed material should be performed on the basis of material Furthermore, the slope of S–N curves is decreased. Never-
data referring to the conditioned state, or if not available, theless, the design of real parts, usually prone to water
fatigue master curves should be modified with reference to absorption, is still possible by taking into account these
the S–N curve of the virgin material in the conditioned state. effects in the use of the S–N master curve.
The presence of water in the matrix does not signifi-
cantly affect the possibility of reprocessing the material,
Acknowledgements
since ground material is usually exsiccated prior to being
fed into the injection machine. However other factors orig-
The authors gratefully acknowledge financial support
inating from service conditions may contribute to the deg-
provided by the Italian Ministry for University and Tech-
radation of the composite and make reprocessing of
nological and Scientific Research (MIUR) under Grant
materials from post consumer waste difficult, namely con-
No. 2003094300 004 (PRIN 2003). They also wish to thank
taminations from solid impurities and service fluids and
Mr. Allevi, Mr. Troiani and Mr. Gornati for help in con-
thermal ageing. Difficulties may arise when trying to deter-
ducting the experiments.
mine the effect of real service conditions by testing materi-
als recovered from post consumer waste, if the history of
the part to be recovered is not known. References
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