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Torres 2003
Torres 2003
take part. Then the mould is cooled down and the part is ex-
The present paper describes the development of a new proces- tracted from it.
sing technology: rotational moulding of natural fibre rein- However, not many fundamental studies have been carried
forced thermoplastics. Different polymer-natural fibre and out to understand the underlying principles that govern this
polymer-flour systems have been characterised. A rotomould- process. In that sense, powder processing of metals and cera-
ing grade of high density polyethylene has been used as the mics has been the subject of more detailed studies and several
polymer matrix for the experiments. Fibres, including jute, si- models have been proposed to explain the different types of
sal and cabuya, as well as wood, pecan and rice shell flour of sintering processes that occur in industrial operations. In the
different types have been used as reinforcements. polymer field, however, there is still discussion whether sinter-
The rotomoulding process for those composite systems has ing or coalescence are the governing processes in the roto-
been studied using an in-house built two-axis rotomoulding moulding technique. Moreover, no consistent models have
rig with variable speed. The final products have been charac- been produced to explain the processes of multicomponent or
terised with special emphasis on estimating the level of disper- multiphase sintering with polymers.
sion of the fibres and their degree of orientation, as well as the The work presented here is part of a long term research pro-
consolidation, sintering and bubble formation processes dur- ject. It studies the possibility of producing single- and multi-
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ing the different stages. Comparisons have been made with layered natural fibre reinforced polymer products with the ro-
other powder processing routes, involving the sintering of fibre tomoulding technique.
(or flour) reinforced polymer particles including compression Natural plant fibres have been used in the past as a reinfor-
moulding. cing material for different types of matrices [1, 2]. In recent
Morphological characterisation techniques have been years, attention has been paid to their use as a reinforcing mate-
adapted to determine the structure-property relationships in rial for thermoplastics. Particularly the automotive industries
these materials at different processing stages. Important im- have shown interest in the advantages that this type of fibre –
provements in the compression strength of the natural fibre re- reinforced systems can provide [1, 2]. The advantages of biofi-
inforced rotomoulded products compared to the unreinforced bres over traditional fibre reinforcements, such as glass fibres,
materials, accompanied of a good dispersion level of the rein- are: low cost, low density (good specific properties), reduced
forcing fibres have been reported. wear in processing equipment, high toughness, biodegradabil-
ity, “ecological friendliness” (since they can be produced from
renewable resources).
Natural plant fibres can be classified, considering their ori-
1 Introduction gin, as follows: a) leaf: sisal, pineaple leaf fibre (PALF), bana-
na leaf fibre; b) bast: flax, ramie, hemp, jute; c) seed: cotton;
Powder processing of thermoplastics is not a new processing d) fruit: coconut, husk.
technique. Powder coating has been used for a long time with
different thermoplastic polymers. The rotomoulding of PVC
plastisols for the production of toys and balls has also been a
common procedure for many years. More recently, the rota- 2 Sintering of Polymer Powder Particles
tional moulding of high density polyethylene has gained con-
siderable importance, due to its proved advantages in the man- Powder sintering has been studied thoroughly for metals, cera-
ufacture of hollow plastic products. Rotational moulding of mics and combinations of these and other materials [3]. How-
plastics, or rotomoulding, starts with loading a mould with ever, not many fundamental studies have been carried out to
polymer powder. Then the mould is rotated in two axes at rela- understand the nature of the underlying processes that take part
tively low speeds (usually 10 to 30 min – 1 among industrial op- during the formation of a dense material when a polymer pow-
erations) while been heated so that particle consolidation can der is sintered, as occurs in the rotomoulding process. Most ex-
perimental studies are based on the original treatment proposed
* Mail address: F. G. Torres, Dept. of Mechanical Engineering, Pon- by Frenkel [4] and modified by Eshelby [5]. In this case, the
tificia Universidad Católica del Perú, Av. Universitaria Cdra. 18. driving forces of the sintering process are the viscous forces
s/n Lima 32, Peru and the surface tension. This leads to a simple equation for the
evolution of the neck formation: Due to the irregular shape of the polymer powders used in
1=2 the experiments described here (Fig. 1.), none of these models
x tC
¼ ; ð1Þ have been verified in the present study.
a ga0
where: a ¼ particle radius, a0 ¼ initial particle radius,
t ¼ sintering time, x ¼ sintering neck radius, C ¼ surface ten-
sion, g ¼ particle viscosity. 3 Powder Processing of Fibre Reinforced Polymers
However, as Oberacker and Thummler point out [3], this and
other analytical models which attempt to describe the sintering The use of polymer matrices in powder form is a manufactur-
process, assume perfectly spherical particles, and the formation ing route that has not received much attention when employing
of a rounded neck between the particles. This has been verified natural fibres as a reinforcement in composites. The only com-
International Polymer Processing downloaded from www.hanser-elibrary.com by Kungliga Tekniska Högskolan on December 8, 2015
not to be the case in real sintering process for metals and cera- mon polymer composites manufacturing techniques in which
mics [3], and more recently for polymers [6, 7]. polymer powders are formed together with fillers and reinfor-
Polymer sintering as occurs in rotomoulding has been stu- cing fibres are compression and transfer moulding of rein-
died by very few authors. The sintering behaviour and the bub- forced thermosets. However, those processes have not been
ble formation process in rotomoulding has been studied by treated as polymer sintering.
Crawford et al. [8, 9]. More recently, Vlachopoulos et al. [6] In the context of rotomoulding, not much has been reported
have stressed the importance of viscoelasticity in polymer sin- on the use of reinforcing fibres or filler materials, even though
tering. They suggest that sintering, as it exists in metals and it is known to the authors that some academic as well as in-
ceramics, does not take actually place with polymers, but it is dustrial organisations have attempted to develop such pro-
coalescence the governing mechanism in the formation of a cesses.
dense polymer bed out of heated polymer particles. Moreover, no theoretical study has been offered yet to de-
Vlachopoulos et al. have used a differential viscoelastic scribe the sintering process of polymer particles in the presence
model (Maxwell model) to describe the sintering process and of reinforcing fibres or fillers. On the other hand, in the metals
have proposed the following relationship, assuming a ¼ ao , and ceramics field, the classification of the different types of
and approximating h2 to ðx=aÞ2 [6]: sintering processes seems to be well established. Thümmler
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3.1 Characterisation of Polymer Particles ments and f) was used exclusively in the compression mould-
ing experiments.
The first step has been the characterisation of the HDPE pow- In all rotomoulding experiments the fibres were used as a
ders used in the rotomoulding and compression moulding ex- discrete reinforcements (5 to 10 mm long) blended with the
periments. Two HDPE powders, natural white and black, have polymer powder. For the compression moulding experiments,
been used in the experiments. Both types were commercial jute fabrics (Fig. 2f) and discrete sisal fibres (Fig. 2a) were
grades available to local rotomoulders. The powders MFI has used.
been measured using a standard Ceast MFI equipment follow- The treatments applied to the fibres included: washing of the
ing ASTM D1238. The test was carried out at 190 °C and with fibres in an alcohol solution for 24 h, application of a disper-
a load of 2.16 kg. The MFIs of the HDPE polymers were 2.8 sion agent (stearic acid) and drying the fibres for 24 h at 65 °C.
and 2.5 for the natural white and black powders respectively.
International Polymer Processing downloaded from www.hanser-elibrary.com by Kungliga Tekniska Högskolan on December 8, 2015
showing most of the fibres close to the specimen inner surface, B) Dou-
ble layer natural fibre reinforced rotomoulded specimen showing good
Fig. 3. Rotational moulding rig used in the experiments fibre distribution across the specimen thickness
Fig. 4. Section of the mould used in the rotomoulding experiments (a 4.3 Characterisation of the Rotomoulded Composites
section of the rotomoulded product is shown in the inside in lighter col-
our) The external appearance of the rotomoulded composites
showed a high variation depending on the type and content of
the reinforcing fibres used in each case. Some of the reinforced
4.2 Study of the Process specimens moulded are shown in Fig. 6. The composite ob-
tained with HDPE and rice shell flour was particularly interest-
The speed in the first axis was varied between 30 and 100 min – 1. ing due to its paper-like aspect. However, its mechanical prop-
These speeds can be considered to be high for an industrial ro- erties were not among the best of the composite systems
tomoulding situation, however due to the small size of the lab studied.
rig used, this range of speeds was adequate for the experiments. Fibre dispersion is a key issue, since it strongly influences
The temperature of the oven was monitored with a thermocou- the reinforcement efficiency in discrete fibre composites. As
ple and during the heating process was in the range 130 to can be observed from Fig. 7a an extremely good level of dis-
220 °C. The samples were in all cases 30 g in weight. The per- persion can be achieved by the rotomoulding process of HDPE
centage of fibres and flour was varied in the experiments be- and treated sisal fibres. It is also important to note that the fibre
tween 0 and 50 %. The matrices used were HDPE in powder mat structure apperas to be quasi-isotropic, which is a desirable
form, both natural and black (with carbon black) as described property in this type of products.
in section 3.1. All fibres and flour used have been treated as The internal and external surfaces of the rotomoulded speci-
mentioned in section 3.2. They have also been pre-dried at mens have been studied using a Zeiss stereomicroscope with
65 °C for 24 h. The polymer powder and the second phase (re- external incidental light. The internal surface of one of the
inforcing fibres or wood and shell flour) were dry blended be- walls of the single layered cylindrical specimens is shown in
fore the rotomoulding tests with the aid of dispersion agents, Fig. 8. As can be seen from the figure, many fibres stick out
such as stearic acid. Then the blended materials were placed in- of the surface, and only a portion of the reinforcing fibres are
side one half of the mould. The mould was then closed and embedded in the polymer matrix, contributing to the reinforce-
placed in the rotomoulding rig, and the process was started. ment of the matrix. This supports the idea of producing multi-
When introducing polymer and fibre together at the begin- layered rotomoulded articles, in which a pure polymer internal
ning of the process, it was found that most of the fibres tend to layer is deposited and sintered on top of the existing polymer –
remain close to the inner surface of the moulded specimen fibre bed, to produce a good internal finish and ensure a full re-
(see Fig. 5A). In order to obtain an adequate fibre distribution inforcing effect of the fibres.
Fig. 9. shows a micrograph of the external surface of one of density of the polymer bed (evaluated qualitatively – using
the two parallel flat areas in the specimens (see Fig. 6). The con- stereomicroscopy – by the void content) was lower than that
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centric circles shown in the picture correspond to the machining found in the fibre reinforced composites. Moreover, a more
traces on the steel mould surface replicated by the polymer when porous structure was found in the flour-filled materials. In gen-
in contact with the mould. A good level of fibre dispersion below eral, the overall sintering behaviour of the polymer matrices
the surface can be appreciated in the figure. A quasi-isotropic fi- used in the experiments, as observed under the microscope, ap-
bre orientation can also be observed in this case. peared to be very similar to that of the unreinforced polymers.
In Fig. 10. it is possible to observe the appearance of bubbles In fact, similar sintering times were determined when using
in the polymer matrix. This corresponds to a high heating/sinter- equal amounts of materials, in both cases, reinforced and un-
ing time (20 min). Fibre degradation was also observed in this reinforced. Therefore from this study it cannot be determined
specimen. In all cases, the sintering times had been long enough whether the presence of a second phase has a significant effect
for achieving almost full density. No porous structures were ob- in the sintering behaviour of a multiphase polymer system.
served under the microscope for the specimens shown in Figs. 7, The mechanical properties of the rotomoulded cylinders
8 and 9. The bubbles appearing in Fig. 10 are not pores remain- were characterised in the compression mode. The samples
ing from an unfinished sintering process, considering that the were placed in an Instron hydraulic universal testing machine
specimen in Fig. 10 had the longest sintering time of all. and compressed in a similar way to plastic pipes (Fig. 11).
In all cases the polymer matrices in the rotomoulded compo- The crosshead speed was 1.3 mm/min. The recorded maximum
sites displayed the same characteristics of the polymer in the forces for the different materials are presented in Table 1. Good
unreinforced mouldings. This was particularly true, for the replicability was found in all cases.
pre-treated fibre reinforced composites with weight contents As can be seen in Table 1, in all cases the reinforced mould-
under 15 %. In the case of the flour-filled composites, the final ings show higher compression forces than the unreinforced
Fig. 8. Micrograph of the inner surface of a Fig. 9. Micrograph of the outer surface of a Fig. 10. Micrograph of the outer surface of a
rotomoulded specimen showing good fibre rotomoulded specimen showing good fibre rotomoulded specimen showing bubbles. The
dispersion with fibres sticking out of the poly- dispersion in the polymer bed. The concentric concentric circles are machining tracks repli-
mer matrix (15 ×) circles are the machining tracks replicated cated from the mould surface (15 ×)
from the mould surface (15 ×)
10 mm) and woven jute fabric. In the case of the fabric rein-
Fig. 11. Compression testing of the rotomoulded products forced composites, only one layer of fabric was placed between
two layers of HDPE natural powder. For the discrete fibre rein-
HDPE. Particularly, the combination of HDPE with 10 % of forced composites, the chopped fibres were placed by hand on
dry sisal, with the use of a dispersion agent (stearic acid) which top of one layer of polymer powder and then covered by a sec-
enhances the fibre dispersion in the matrix, shows the highest ond layer of the same powder.
compression force (1000 N). This corresponds to an improve- A manual lab press equipped with independent temperature
ment of 53 % of the compression force of the unreinforced controllers for each platen has been used for the experiments
polymer. (Fig. 12). Unreinforced and composite plates were produced
It was also interesting to observe that the fibre reinforced roto- with a simple male-female mould. The moulding temperature
moulded specimens showed a good degree of recovery after the was 180 °C.
compression tests, whereas, on the other hand, the unreinforced The specimens produced by compression moulding were ex-
polymer specimens showed permanent deformations. This may amined using stereomicroscopy. Fig. 13 shows the cross sec-
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indicate that a great part of the energy absorbed by the fibre rein- tion of a fabric reinforced compression moulded specimen
forced specimen is actually stored elastically by the reinforcing using a jute fabric as a reinforcement. The polymer matrix
mat structure. This is in agreement with results obtained for dis- was found to be well consolidated and approaching full density,
crete long glass fibre (LGF) composites reported by Torres et al. showing a similar sintering behaviour to the compressed un-
for the thermoforming process [10 to 12]. reinforced polymer powders. The fabric was however only im-
The weight variation in the specimens has been measured pregnated superficially.
after rotomoulding. As can be seen in Table 2, a considerable Fig. 14 shows the cross section of a discrete fibre reinforced
weight loss has been found when using sisal fibres without compression moulded specimen containing sisal fibres. The
pre-drying. When using dry fibres a weight gain of 1.6 % has polymer also seemed well consolidated. The fibre dispersion
been recorded, thus indicating that the composite moulding is was limited compared to the rotomoulding process and the
taking up moisture from the environment after processing. As same was valid for the fibre orientation. This is due to the re-
can be inferred from the results, weight measurements with stricted flow and movement of the fibres that takes part in the
natural fibre reinforced polymers can be complicated due the compression moulding process compared to the rotomoulding
hydrophilic nature of the fibres. process. In the rotomoulding process the fibres are organised
during the entire consolidation process, which allows for a bet-
ter fibre distribution and a more controlled fibre orientation.
5 Compression Moulding Since the rotation used in these experiments was biaxial, fibre
orientation tends to be quasi-random.
For comparison purposes, compression moulding experiments
have been performed. The same polymer powders as in the ro-
tomouding experiments have been used. Two different types 6 Conclusions
of reinforcements have been used: chopped sisal fibres (5 to
It has been shown from the present studies, that it is possible to
produce discrete natural fibre reinforced rotomoulded products
Reinforcing fibre Fibre content Max.
showing a good level of fibre dispersion. These composites
w/w force
% N show good mechanical properties (as verified by compression
tests) with regard to the unreinforced polymers. Moreover, the
Sisal (no pre-drying) 10 810
fibre mats tend to be quite stable under large deformations
Sisal (dry) 15 700 and allow for a considerable recovery of the deformation. The
Sisal (dry) + Stearic acid 10 1000 levels of fibre dispersion obtained when pre-treating the fibres
Rice shell flour 5 680 were very good for this type of discrete reinforced materials.
Unreinforced HDPE 0 650 In addition, the fibre orientation in the mats corresponds to a
quasi – isotropic structure. The examination of the inner sur-
Table 1. Maximum force recorded in the compression test face of the single-layered rotomoulded specimens shows that
a large proportion of the fibres stick out of the polymer matrix. Fig. 14. Cross section of a discrete reinforced compression moulded
This decreases the reinforcing efficiency of the fibres and gives composite (15 ×)
a rough internal finish. In order to obtain an optimal reinforce-
ment efficiency and a good internal surface finish, an extra in-
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