Composites: Part A 32 (2001) 12711279

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Natural bre reinforced sheet moulding compound

B. van Voorn*, H.H.G. Smit 1, R.J. Sinke, B. de Klerk
Polymers, Composites and Additives, Agrotechnological Research Centre (ATO), Wageningen University Research Centre, P.O. Box 17, 6700AA Wageningen, The Netherlands Revised 24 April 2001; accepted 18 May 2001

Abstract This paper describes a newly developed system, which enables utilisation of short ax bres for SMC (Sheet Moulding Compound) production. It is shown that by using an evenly distributed layer of short dried ax bres, after controlled impregnation and maturation, a homogeneous ow of the prepreg in the mould is obtained, and accordingly a ax bre reinforced SMC can be produced. Mechanical data indicates that for applications designed with respect to stiffness, ax bre reinforced SMC materials compete with glass bre SMC, especially when the bre length exceeds 25 mm. q 2001 Elsevier Science Ltd. All rights reserved.
Keywords: A. Fibres; A. Prepreg; B. Wear; B. Mechanical properties; Sheet moulding compound

1. Introduction Nowadays a growing interest exists for the use of natural bre reinforced composites (NFRC) in the automotive industry [14]. NFRC's exhibit several advantages compared to glass bre reinforced composites (GFRC), such as low density and low equipment wear. On top of this, damaged NFRC are non-abrasive. Furthermore, cellulosic bres (like jute, sisal, abaca, ax) are relatively cheap and obtained from renewable resources. This project [5] aims for replacement of glass bres in Sheet Moulding Compound (SMC) by natural bres in the transportation sector. These products comprise different kinds of bodywork, like spoilers, fenders, funnels, etc. and gain more and more interest by the transportation industry because of their specic properties. An additional benet of NFRC with respect to GFRC is its end-of-life scenario. Due to European legislation on waste dumping, NFRC exhibit the advantage of being combustible, this in contrast to GFRC. SMC is a compression moulded short bre reinforced thermoset composite which is produced in a two-step production process [6]. The rst step is the preparation of the so-called prepreg. A SMC-prepreg is a stiff sheet consisting of components like UP resin, reinforcing bres, inorganic llers and catalyst, but also, which is character* Corresponding author. Tel.: 131-317-477532; fax: 131-317-475347. E-mail address: b.vanvoorn@ato.dlo.nl (B. van Voorn). 1 Present address: Acheson Industries, Scheemda, The Netherlands.

istic for SMC, ingredients like release agent, anti shrink agent and thickener. One of the essential demands in the SMC technology is the homogeneous ow of the prepreg during the second step of the process, which is compression moulding, into the desired shape [6,7]. The prepreg must remain homogeneous during ow to the extremities of the mould. The thickener, usually MgO, raises the viscosity and thereby not only simplies the handling of the prepreg, but increases also the viscosity during the second step of the process. The increased viscosity enables the ow of the reinforcing bres with the resin throughout the mould. After moulding a homogeneous material is formed with uniform properties [8]. Due to their intrinsic properties [2,9], ax bres behave differently from glass bres and up to now limited data are published on ax bre SMC (FFSMC) [10]. In this work a newly developed system to use short ax bres for use in SMC production is investigated. The essential parameters are: the inuence of moisture content of the ax bres upon maturation; the inuence of ax bres upon thickening; the homogeneous ow of the bres with the matrix during compression moulding. In this paper the mechanical properties of the FFSMC are compared to glass bre SMC (GFSMC). Inuence of bre and ller percentage on the tensile, exural and impact

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properties is determined as well as the inuence of the bre length on the exural properties. 2. Experimental 2.1. Materials A standard SMC resin formulation (paste) with varying content of ller and thickener is used and kindly supplied by Wientjes B.V. Emmen, The Netherlands. The reinforcing bre in the NFSMC is ax. The ax bres used for this research are dew-retted, scutched bres and cut to desired lengths. Most of the research is performed using 6 mm bres, but also 13, 25 and 38 mm are used. 2.2. Composite preparation The intrinsic tensile strength of several bres is determined using a stelometer according to ISO 3060. Mechanical properties of the bres are also tested under severe conditions regarding temperature and moisture. Both ax and sisal bres are tested in a temperature range of 280 to 708C and relative humidities (RH) ranging from 22 to 98% RH. For the preparation of prepregs, dew-retted, scutched ax bres are cut to desired lengths, usually 6 mm (otherwise 13, 25 or 38 mm). Glass bres used in this research were pre-cut at 25 and 50 mm (Wientjes

Emmen B.V.). Before impregnating the ax bres with the resin paste the bres are evenly distributed in a box, to form a uniformly distributed layer of bres, by using a rotator and sieve for bre lengths up to 6 mm, as depicted in Fig. 1. Longer bres need a different method to form a uniform bre layer. ATO developed a bre dryer which is a 40 m long tube through which (hot) air is blown. The air stream loosens the bres and at the end of the tube the bres are separated from the air stream by a cyclone. Fibres from the cyclone do not stick together and this results in a nicely distributed bre layer. This bre layer is dried overnight at 708C before impregnation. The required amount of paste is mixed and evenly distributed onto two Polyamide (PA) sheets. The dried ax bres are directly transferred from the box to the PA sheets. The bres are impregnated with the paste by passing the prepreg through a series of 4 compaction rolls, in which each roll increases the pressure on the prepreg. To avoid water uptake of the bres in the prepreg, the prepreg is placed in a PE bag, sealed and left to mature for approximately one week at room temperature. After maturation the prepregs are compression moulded in a round mould B 22 cm or a rectangular mould 40 30 cm at a temperature of 1408C and a pressure ranging from 3.514 MPa. The curing time is varied from 26 min. Flow of the bres is determined by lling the mould with 70% of its area covered with prepreg, thereby inducing ow. Maturation tests are performed on a so-called Renol-mould.

stirrer

fiberfeed Swirling fibers

Stirring blade sieve

fiberlayer PP foil

Fig. 1. Schematic drawing of the bre distributor.

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Fig. 2. Tensile strength of several natural bres and regenerated cellulose as a reference.

A Renol-mould is a round mould with spiral openings in the male side of the mould. During compression moulding the paste and bres are allowed to ow in these spiral openings. The distance the bres and paste travel in these spiral determines the amount of maturation of the system. Although this test is not quantitative, it gives a good insight in the maturation characteristic of a certain prepreg. Samples were tested on a Zwick tensile tester according to ISO 527-4, ISO 178 to determine tensile and exural properties. Charpy impact properties were tested according to ISO 0179 on a CEAST RESIL machine. 3. Results and discussion Several parameters are important when dealing with SMC and especially NFSMC. These parameters are the nature of the bres, bre distribution, moisture, impregnation, maturation and compression moulding. Each of these will be discussed separately. Inuence of bre

and ller percentage on the mechanical properties like tensile, exural and impact properties are discussed, as well as the inuence of bre length on the exural properties. 3.1. Fibres In this study predominantly ax bres are used to develop a NFSMC system. From Fig. 2 can be seen that ax bres exhibit very good tensile properties as compared to other natural plant bres. This together with a good availability and competitive price in Europe makes ax a very promising bre for future use of NFSMC. The performance of ax bres and sisal is also tested under more extreme conditions. The inuence of relative air humidity (% RH) and temperature on the strength of the ax bres is measured and shown in Figs. 3 and 4. From Fig. 3 it can be concluded that the relative humidity affects the strength of the bres. Under standard conditions, ax is measured at 50% RH, but it shows that for both ax and sisal a maximum exists at 70% RH. Measurements over the humidity range of

1200

1000 Tensile strength (MPa)

800

600

400 flax 200 sisal

0 10 20 30 40 50 60 70 80 90 100 110 Relative hum idity (%)

Fig. 3. Tensile strength of ax and sisal bres under different relative humidity (% RH).

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1000

Tensile strength (MPa)

800

600

400

200

flax sisal

0 -100

-80

-60

-40

-20

20

40

60

80

Tem perature (C)

Fig. 4. Tensile strength of ax and sisal bres under different temperatures.

2298% RH show no severe loss of tensile strength of both ax and sisal, when compared to the value at 50% RH. In Fig. 5 the water uptake at different relative humidities is shown. The environmental temperature has a limited effect on the tensile strength (See Fig. 4). A decrease in the performance of both ax and sisal bres is observed near 2208C and a peak can be seen near room temperature, with a small loss in tensile strength at higher temperatures, which is probably due to the loss of water.
16.0

3.2. Fibre distribution In contrast to glass bres, ax bres tend to entangle and stick together. In order to obtain an evenly distributed layer of single separate bres with uniform length a bre distributor is used. By passing the bres through a sieve (with 5:6 5:6 mm2 openings) using a rotator the bres get separated from each other (see Fig. 1). The longer (.6 mm) and entangled bres stay behind in the apparatus. The bre layer then consists of randomly orientated separate

14.0

12.0

10.0

% water

8.0

wt% water at 70C, after conditioning at 90% RV, 20C wt% water at 90%RV, 20C, after drying at 70C

6.0

4.0

2.0

0.0 0 1 2 3 4 5 6 7

Time (hrs)
Fig. 5. Moisture uptake and release of dew-retted ax.

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Fig. 6. Roller with pressure gradient.

bres and these can separately be impregnated with the resin paste. Larger openings of the sieve do not necessarily make the use of longer bres possible. Actually, a bre length of 6 mm is found to be the maximum bre length that can be distributed evenly using this technique. For bres longer than 6 mm the ATO bre dryer is used, which makes it possible to evenly distribute bres with a maximum length of 38 mm. 3.3. Moisture Moisture has a negative effect on the maturation of the prepreg and degree of thickening and hence the bre ow during compression moulding [11]. Standard GFSMC is allowed to contain a maximum of 0.5 wt% water. As can be seen in Fig. 5, at room temperature ax bres contain approximately 1214 wt% water, of which 2% is bound to the bres [12]. The latter cannot be removed reversibly by means of drying. After drying at 708C for 6 h the bre are dry (2 wt% moisture), the uptake of water at room temperature starts very quickly, so there is only limited time to transfer the dried bre layer from the oven onto the sheets (see Fig. 5).

3.4. Impregnation Contact and interaction between bres and resin is of crucial importance for the optimum performance of a composite. It is known that composite materials perform best when all bres are in contact with the resin. In this way, the resin is able to transfer the applied forces to the bres most optimally. In this regard, it is very important to achieve maximum impregnation of resin and bres. Several common techniques are used, like compaction rolls, cold pressing, but the roller depicted in Fig. 6 gave the best impregnation results. This roller makes use of four compaction rolls placed sequentially enlarging the pressure from roll to roll. Adjustments to the distance between the rolls can be made to increase the pressure even more. 3.5. Maturation Final thickening is a timetemperature dependent reaction usually requiring several days, before the prepreg is ready to be moulded. This reaction is inhibited by water and therefore it is necessary to dry the bres in advance. The maturation (thickening) is needed for the operator to handle the prepreg, cut them into desired shapes and placing

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Fig. 7. Renol Mould with its spiral openings.

them in the mould. Depending on the amount of inorganic ller (e.g. chalk), bre and thickener percentages, the maturation of the prepregs takes 411 days and can be stored up to six months, see Table 1. Incomplete maturation yields inhomogeneous SMC's, i.e. the bres do not ow with the paste as is tested with the so-called Renol mould. See Fig. 7. The Renol mould is a spherical mould with two spiral openings. The length of the pathway the material has travelled during compression moulding is a measure for the ow. Experiments have shown that drying of the bres prior to impregnation is necessary to obtain ow. Also, when using the bres as cut, without using the distributor, the entanglements in the bres prevent homogeneous ow and hence prevent producing a homogeneous SMC material.

3.6. Compression moulding In the nal step of the SMC-process, which is compression moulding, the actual product is formed. Temperature, pressure and time are varied. From the data it became clear that a temperature of 1408C and times varying between 2 6 min gave best results. The duration of the compression moulding step depends on the thickness of the prepreg. Compression moulding pressures between 3.5 and 14 MPa were used to set the composite. Higher viscosities made it possible to press at higher pressures. 3.7. Mechanical properties In this study three mechanical properties are studied in detail. These are tensile, exural and impact (Charpy) properties. Both strength and modulus are determined in tensile and exural tests. Effects of bre percentage, ller percentage, bre length are determined. All experiments are carried out using 6 mm ax bres, unless otherwise stated. In Fig. 8 can be seen that both ax bre and inorganic ller cause an increase of the E-modulus and strength of FFSMC. As expected, in general can be said that increasing the amount of bre and ller will increase the tensile properties. The exural properties show similar effects. See Fig. 9. With increasing bre and ller percentage, both the modulus and strength increase. The amount of ller has no signicant effect on the impact strength of the FFSMC, however an increase in the

Table 1 Minimum maturation time required. After 14 days the maturation was stopped, due to insufcient thickening (n.d.: not determined) Fibre (wt%) 15 15 15 15 15 15 20 20 Filler (wt%) 21 21 38 38 38 48 38 38 Thickener (wt%) 1.5 4 2 3 4 1.5 4 4 Maturation time (days) n.d. 8 7 6 4 10 8 11

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Fig. 8. Tensile properties of FFSMC. The columns on the left are the E-moduli, on the right the tensile strengths.

Fig. 9. Flexural properties of FFSMC. The columns on the left are the moduli, on the right the exural strengths.

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Fig. 10. Impact properties of FFSMC.

amount of ax bres causes an increase in impact strength, see Fig. 10. When the inuence of bre length is regarded in NFSMC, a rather profound effect is to be observed. Fibre lengths that were used are 6, 13, 25 and 38 mm. From Fig. 11 can be concluded that the bre length has a large inuence on the exural properties of the NFSMC. Apparently, the critical bre length is larger than 6 mm and may be somewhere around 25mm. This is also the minimum bre length used in commercial GFSMC. These experiments are performed using 22 vol% ax bres and 38 vol% chalk as a ller. When compared to GFSMC, (see Table 3) the stiffness of FFSMC shows similar or even better values. However, the tensile and exural strength of FFSMC are slightly lower,
15 Flex. Modulus (GPa) in u 12 9 6 3 0 0 10 20 30 Fibre length (mm) 40 200 175 150 125 100 75 Flex. Strength (MPa) in l

while the impact properties are substantially lower then those for GFSMC. This is due to several factors. First, the intrinsic tensile properties of glass bres are superior to (technical) ax bres. (See Table 2). This immediately explains the difference in tensile strength between GFSMC and FFSMC according to the rule of mixtures. Secondly, most of the testing is performed using 6 mm natural bres. When using bre lengths exceeding 25 mm in FFSMC the mechanical properties are comparable to GFSMC. Third, the impact strength is substantially lower, probably because of the anisotropic
Table 2 Comparison of the intrinsic properties of E-glass and ax bres Fibre E-glass Flax Density (kg/m 3) 2500 1400 E-modulus (GPa) 73 80 Tensile strength (MPa) 2500 800

Table 3 Comparison of GFSMC and FFSMC SMC E-modulus (GPa) Tensile strength (MPa) Flexural Modulus (GPa) Flexural strength (MPa) Impact strength (KJ/m 2) GFSMC 811 3575 711 70160 4070 FFSMC 712 4080 712 83144 73

Fig. 11. Inuence of bre length on the exural properties of FFSMC.

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nature of the ax bre and the bre length used. It is known that isotropic bres, like glass bres, perform better on impact than anisotropic bres like all natural bres. The anisotropy gives the bres very good tensile properties, but affects its impact properties. To show that it is possible to use FFSMC instead of GFSMC a pilot production trial is carried out. Several trials on one type of commercial moulded product using three different formulations, all showed that a homogeneous product can be made from FFSMC, in which the ax bres have own into all the extremities of the mould. Weight savings of 1120% can be achieved when, respectively, 1530 vol% ax bres are used instead of glass bres. Table 3 shows a comparison between GFSMC and NFSMC using ax (FFSMC). This table shows literature data on GFSMC and the experimental data on FFSMC. The modulus of both tensile and exural tests are comparable or even slightly better for FFSMC. The tensile and exural strength for FFSMC are slightly lower but comparable to GFSMC. Currently research is performed to enhance the impact properties of FFSMC. 4. Conclusions In this work a new system for producing ax bre SMC is developed. Flax was chosen to be the bre for this research, because of its tensile properties, price and availability. Natural bres behave different in different atmospheric conditions but even under extreme conditions, the bres show good properties. Development of a bre distributor, good impregnation of the prepreg between compaction rolls, drying the bres prior to impregnation and monitoring the maturation led to ow of the bres to the extremities of the mould during compression moulding, which resulted in a homogeneous ax bre SMC-product, which was 1120% lighter than the same product for GFSMC. From the mechanical data it is shown that varying the bre and ller percentages and bre length led to the result that the stiffness of ax bre SMC is equal to or even slightly better than the stiffness of glass bre SMC. Increasing the bre length led to an enormous improvement of the tensile and exural strength which resulted in comparable results to that of GFSMC. As expected beforehand, the impact properties are lower than that of GFSMC. This is partly due to the anisotropic nature of the ax bres in contrast to the isotropic nature of the glass bres. From this work it is concluded that for products

designed with respect to stiffness and to a lesser extent strength ax bre SMC material can compete with glass bre SMC material. Acknowledgements This research is performed in the framework of the `Biolicht'-project which is carried out by ATO in cooperation with Wientjes. Emmen B.V, Energy Research Centre The Netherlands ECN, Delft University of Technology, Kiem, Ceres and Cintec/Focwa. This project is funded by the Dutch Ministry of Economic Affairs and the Dutch Ministry of Education, Culture and Science by means of an Economy, Ecology and Technology (E.E.T.) subsidy. References
[1] Canche-Escamilla G, Cauich-Cupul jI, Mendizabal E, Puig JE, Vasquez-Torres H, Herrera-Franco PJ. Mechanical properties of acrylate-grafted henequen cellulose bers and their application in composites. Composites 1999;30:34959. [2] Sanadi AR, Prasad SV, Rohatgi PK. SEM observations on the origins of toughness of natural bre-polyester composites. J Mater Sci Lett 1986;395:396. [3] Mitra BC, Basak RK, Sarkar M. Studies on jute-reinforced composites its limitations and some solutions through chemical modications of bers. J Appl Polym Sci 1998;67:1093100. [4] Peijs T, Garkhail S, Heijenrath R, van den Oever M. Thermoplastic composites based on ax bres and polypropylene: inuence of bre length and bre volume fraction on mechanical properties. Macromol Symp 1998;127:193203. [5] This project is carried out in collaboration with Wientjes Emmen B.V. Delft University of Technology Energy Research Center, The Netherlands (ECN) Ceres B.V. FOCWA/Cintec and KIEM. [6] Sawallisch K. Compounding of sheet molding compound. Polymplast Technol Engng 1984;23(1):136. [7] Castro JM, Grifth RM. Sheet molding compound compressionmolding ow. Polym Engng Sci 1989;29(10):6328. [8] Kim KT, Jeong JH, Im YT. Effect of molding parameters on compression molded sheet molding compound parts. J Mat Proces Techn 1997;67:10511. [9] van Hazendonk JM, Reinerink EJM, de Waard P, van Dam JEG. Structural analysis of acetylated hemicellulose polysaccharides from bre ax (linum usitatissimum L). Carbohydr Res 1996;291:14154. [10] Kessler RW, Kohler R. New strategies for exploiting ax and hemp. Chemtech 1996;34:42. [11] Blancon R, Martinez-Vega JJ, Merle G, Revellino M, Camino G, Ya. Polishchuk A, Luda MP. Durability of sheet molding compounds: inuence of hydrothermal aging on morphology and molecular mobility at microscopic scale. Polym Engng Sci 1997;37(10):172231. [12] Hatakeyama T. Effect of bound water on structural change of regenerated cellulose. Makromol Chem 1987;188:187784.