Applied Composite Materials 7: 403414, 2000. 2000 Kluwer Academic Publishers. Printed in the Netherlands.

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Mechanical Properties of Natural Fibre Mat Reinforced Thermoplastic

KRISTIINA OKSMAN
SICOMP AB (Swedish Institute of Composites), Box 271, SE-941 26, Pite, Sweden Abstract. The use of natural bres instead of man made bres, as reinforcements in thermoplastics, gives interesting alternatives for production of low cost and ecologically friendly composites. In this work different commercially available semi-nished natural bre mat reinforced thermoplastics (NMT) composites have been studied. Mechanical properties and microstructure of different NMT composites were investigated and compared to conventional GMT (glass bre mat reinforced thermoplastic) composites and pure polypropylene (PP). The study included also NMT composites manufacturing processing parameters as processing temperatures and pressure during compression moulding. The results showed that NMT composites have a high stiffness compared to pure polymer and the NMT with a high bre content (50% by weight) showed even better stiffness than the GMT. The GMT composites had superior strength and impact properties compared to the NMT which might be due to the relatively low strength of the natural bres but also to poor adhesion to the PP matrix. The NMT materials showed a large dependence on direction and are therefore believed to have more bres oriented in one direction. The stronger direction (0 ) of the NMT was in some cases as much as 45% better than the 90 direction. Key words: ax bres, natural bres, thermoplastics, tensile properties, impact properties, anisotropy, electron microscopy, morphology, compression moulding, processing.

1. Introduction During the last few years there has been an increasing environmental consciousness, which has increased the interest to use natural bres instead of man made bres in composite materials. Therefore several manufacturers have started to produce semi-nished NMT materials. The advantages using natural bres instead of glass bres are low density, lower price, low abrasive wear and they are virtually available everywhere. Further the natural bres are recyclable, biodegradable and carbon dioxide neutral and can be energy recovered in an environmentally acceptable way [13]. The natural bres normally involved in these kinds of materials can be for example ax, and the matrix is usually polypropylene (PP). The commercially available NMT materials are nonwoven bre mats melt impregnated by polymers in the form of sheets but also like a nonwoven bre mat where the ax and polymer bres are mixed together in the form of needle punched bre mats. During processing the mats or sheets need to be heated at rst to the melting temperature of the polymer matrix, and then compression moulded to products.

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Several investigations have been made to study the potential of natural bres as reinforcement in thermoplastics [16]. The results have shown that natural bres have potential to be used as reinforcement for plastics but they do not attain the strength level of glass bre reinforced plastics [24]. Mieck et al. [2, 3] showed that when ax bres were used as reinforcements in thermoplastics (PP) the modulus was increased to the level of glass bre reinforced thermoplastics. Heijenrath and Peijs [4] reported that NMT composites made by lm stacking method resulted in composites with comparable stiffness to conventional GMT composites while the strength of NMTs was lower. It is well known that the stress transfer efciency between natural bres and synthetic polymers is poor due to incompatibility between the polar and hydrophilic bre and nonpolar and hydrophobic polymer [68]. Several investigations have been made to study the adhesion between natural bres and synthetic polymers and the results showed that the composite strength and toughness are signicantly improved when coupling agents are used [3, 58]. Possible applications for NMT composites can for example be door panels, headliners, sun visors, spare-tire covers, seat foundations, instrument panels in automotive industry. Non-automotive applications can be for example oor boards, boards for acoustic damping, shipping crates, pallets and furniture. The objective of this work was to investigate processing parameters, mechanical properties and morphology of different semi-nished NMT composites and compare those with conventional GMT.

2. Experiments 2.1.
MATERIALS

Materials used in this study are semi-nished NMT from different manufacturers where two different types of processing techniques have been used: 1. PP melt impregnated bre mat, available as semi-nished product in the form of sheet. 2. Nonwoven of PP bres and ax bres, available as semi-nished product in the form of needle punched bre mat. The advantages of using melt impregnated NMT compared to needle punched mats can be lower moisture uptake during storing and in applications due to complete penetration of the polymer, material ow during compression moulding, easier handling and lower transportation cost. The disadvantages are lower bre content than in needle punched mats. Further, it is believed that the materials are not isotropic which results in different mechanical properties in different directions. The needle-punched mats have long bres which are mostly oriented in one direction (machine direction) while the melt impregnated materials are expected to

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Table I. Sample codes of the various NMT composites Material types, bre fraction (% by weight), density and approximate price. Materials and codes PP Symalit (S) Isosport (I) Danax (D) Mhlmeier (M) Symalit (GMT) Fabrication method melt impregnated melt impregnated needle punched needle punched melt impregnated Fibre content by weight (%)(a) 25 37 50 50 40 Density (g/cm3 ) 0.90 1.00 1.04 1.16 1.13 1.24 Price (DM/kg) 5.4 4.7 3.5 6.5 6.0

a Data from the manufacturer.

Figure 1. Processing steps of semi-nished NMT materials.

be more isotropic but the bres are oriented due to the ow during compression moulding. The composition of the studied materials is shown in Table I. Tested NMT composites were from Symalit AG, Switzerland; Isosport, Austria; Danax, Denmark and Mhlmeier GmbH, Germany. According to supplier data, the NMT materials are reinforced with ax bres and the bre content is varying between 2550 wt%. The GMT had a glass bre content of 40 wt% and was melt impregnated and supplied from Symalit GMT, Lenzburg, Switzerland. The density of compression moulded materials was measured by using a standard test method for plastics (Accupyc 1330). 2.2.
MANUFACTURING COMPOSITES

The processing of the semi-nished NMT materials is made through four steps (shown in Figure 1): 1. 2. 3. 4. Cutting blanks of the sheets (or nonwoven bre mats). Heating the blanks above PP melting temperature. Transport from oven to the press. Moulding of the heated materials by compression moulding.

Rectangular blanks with the width of 350 mm and the length of 450 mm were heated in a combined hot air and infrared (IR) oven using a temperature range of 200220 C and afterwards quickly moved to the conventional hydraulic compression moulding press (Fjellman Press AB, Mariestad, Sweden, capacity of 3100 kN).

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The needle punched mats of PP and ax bres were difcult to heat without burning the material and were therefore contact heated between thick aluminium plates to the temperature of 195200 C. The temperature was controlled by a thermocouple placed between the nonwoven mats during heating. The materials were then compression moulded. This kind of materials can also be heated by blowing hot air through the mats, which is a much quicker way to heat the material than contact heating. The pressure was between 8 and 12 MPa depending on the type of NMT. Melt impregnated NMTs were compression moulded using lower pressure while the needle punched mats need a higher pressure to get a uniform material. Moulded composites had a size of 350 450 mm and thickness between 2.65 mm. The melt impregnated NMTs can ow during the moulding as GMT but the needle punched NMT did not ow due to needle punched structure. All materials had a weight between 700800 g. 2.3.
MECHANICAL TESTING

Tensile testing of the specimens was performed on an Instron test machine (model 8510) using a crosshead speed of 2 mm/min. Samples for the tensile testing were cut to the width of 30 mm and length of 250 mm. The thickness varied between 2.6 to 5 mm. Izod impact testing was performed according to ASTM D 256 on a Karl Frank GmbH impact tester. Test samples for impact testing were machined with a milling cutter. At least 5 specimens of every composition were tested in 0 and 90 directions. The stronger direction is called 0 . 2.4.
MICROSCOPY STUDY

Fractured surfaces of Izod impact specimens were sputter coated with platinum and examined using a Jeol JSM-5200 scanning electron microscope (SEM) at an acceleration voltage of 20 kV. 3. Results 3.1.
COMPOSITE MECHANICAL PROPERTIES

The mechanical properties of the composites obtained from tensile and impact tests are summarised in Table II. Typical tensile curves for tested materials are shown in Figure 2. The curves of needle punched materials, Mhlmeier and Danax follow each other quite well until the break of Danax. The melt impregnated NMT shows similar curve shape. The maximum tensile stress of the NMT composites is shown in Figure 3. It can be seen that it is increased with increased bre content. The tensile stress is shown to be strongly dependent on the direction of the materials and all materials have higher stress in the 0 direction. GMT is less anisotropic compared to

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Table II. Mechanical properties of different commercially available NMT composites, GMT and pure PP.a Tensile properties Composite Dir. Strength (MPa) 28.5 0.6 30.8 0.5 21.3 0.9 34.7 1.8 26.1 2.1 40.2 1.7 35.3 0.8 56.4 2.2 31.1 0.9 77.2 4.4 74.9 7.5 Modulus (GPa) 1.5 0.1 4.6 0.6 2.9 0.3 5.2 0.4 3.9 0.9 6.5 0.4 5.0 0.5 6.3 0.9 3.8 0.4 5.4 0.3 5.1 0.4 Izod impact properties Elongation (%) 1.2 0.1 1.4 0.1 1.2 0.1 1.4 0.5 1.4 0.1 2.2 0.4 1.9 0.1 2.2 0.3 1.8 0.1 1.8 0.1 Notched Unnotched - - - - - - - ( J/m) - - - - - 24 1 70 6 38 0 83 6 49 8 403 23 266 14 194 7 150 9 410 75 553 81 129 8 66 5 149 14 100 13 751 122 450 35 386 24 265 23 717 91

PP S I D M GMT

0 90 0 90 0 90 0 90 0 90

a Standard deviations in parentheses.

Figure 2. Typical tensile test curves for the studied materials.

NMT. The melt impregnated NMTs have 25% to 30% better tensile stress in 0 direction, Danax about 10% and Mhlmeier about 45%. The tested materials did not reach the level of GMT, which was expected due to higher strength of glass bres, 3400 MPa, compared to ax bres about 7501000 MPa [2]. It should be mentioned that the NMT with the bre content of 50 wt% has a tensile strength of 57 MPa, which is twice that of pure PP, 29 MPa.

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Figure 3. Tensile strength of different NMT composites compared to conventional GMT and pure PP.

Figure 4. The elongation at break of the NMT composites compared to the GMT and pure PP.

The elongation at break in Figure 4 shows that the melt impregnated NMT has a lower elongation at break than needle punched NMTs and GMT. The maximum strain is better in 90 direction for all NMT while the GMT have the same strain values in both directions. Figure 5 shows that stiffness of the NMT composites with higher or at least the same bre content by weight as GMT is comparable with the glass bre composites, it is even higher for NMT with 50 wt% ax bre. The modulus for the single ax bres is about 100 GPa, which is better than glass bres [9]. The 0 direction is stiffer for all NMT material and seems to have especially strong effect for Symalit and Mhlmeier. Higher modulus in 0 direction indicates that the bres are more oriented in this direction.

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Figure 5. Stiffness of different NMT composites compared to GMT and pure PP.

Composites impact properties are shown in Figure 6. Izod impact tests showed that NMT composites have inferior impact properties compared to GMT except Danax in 0 direction. In notched samples both NMT and GMT had better impact strength than pure PP. Generally, the impact strength of NMT composites was improved with increased bre content and 0 direction except in the case of unnotched pure PP samples. Tensile and impact strength indicates that the bre-matrix adhesion is poor in the NMT materials. The natural bres can have wide variations in the quality but strength and E-modulus are depending on the form of the bres. Natural bres are usually as bre bundles where the individual bres are bonded together with lignin and/or pectin. The bre bundles have lower mechanical properties than individual bres due to the low bonding strength between the individual bres. We have very little information about the bre quality in the composites used in this work. For example, the natural bres in these kinds of technical applications may well be rest products from textile industry or other low quality bres.

3.2.

COMPOSITE MORPHOLOGY

Scanning electron microscopy of fractured surfaces of different NMT and GMT composites were made to study the morphology and adhesion between the bres and the matrix. Generally, the fracture surfaces of the NMT composites were not as sharp as the GMT fracture surfaces. Figure 7(a) shows a typical fracture surface of NMT composites (S) with a bre content of 25 wt%. It can be seen that there is a lot of bre pull-outs and that the bres are mostly as bre bundles. Figure 7(b) shows a more detailed micrograph of the composite structure. It can be seen that there appears to be poor adhesion

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(a)

(b)
Figure 6. Izod impact properties of (a) notched and (b) unnotched samples.

between the bre bundles and the PP matrix. The surface of the bre bundle is clean and it is also possible to see where the bres have been located before fracture. Figure 8(a) shows an NMT composite (I) with 37 wt% bre content and compared to Figure 7 it has higher bre content. It is again possible to observe many bre pull-outs indicating poor adhesion. Compared to the micrographs in Figure 7 there are more individual bres in these composites. In (b) a more detailed micrograph of the interface shows that the bre surfaces are clean. At larger magnication there were voids visible between the bre and matrix.

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(a)

(b)
Figure 7. Scanning electron micrographs of the fracture surface of a NMT composite (S) with 25 wt% ax bre: (a) overview; (b) detail.

For the NMT composite with a bre content of 50 wt% it was impossible to study the interface region between the matrix and the bres. The bres pull-outs are so long and so many that it was difcult to see any matrix. Figure 9(a) shows that the bre content (by volume) of the GMT is low compared to the NMT in Figure 8 even if the composite has almost the same bre content by weight. The difference is explained by the higher glass bre density, which is about 2.6 g/cm3 compared to natural bres 1.41.5 g/cm3 .

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(a)

(b)
Figure 8. Scanning electron micrographs of the fracture surface of NMT composites (I) with 37 wt% ax bre: (a) overview; (b) detail.

It is also possible to see that the adhesion between glass bres and PP matrix is poor, there are a lot of long pull-outs, the interfacial region shows voids and the bre surfaces are clean. 4. Conclusions The main objective of this study was to investigate the mechanical properties and morphology of four different commercially available semi-nished NMT composites and compare these with conventional GMT and the pure polymer matrix.

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(a)

(b)
Figure 9. SEM micrographs of the fracture surface of a GMT composite with 40 wt% glass bre: (a) overview; (b) detail.

Processing parameters for melt impregnated semi nished NMT showed to be similar to GMT materials, while the needle punched materials need to be contact heated and need longer heating time and also higher pressure during compression moulding. The material ow during compression moulding was good for melt impregnated materials, needle punched materials did not show any ow. The results of mechanical tests show that the stiffness of NMT composites is comparable with conventional GMTs when the bre content is higher or at least as high as the glass bre content by weight. But also that the NMT composites

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properties are highly anisotropic, 0 direction (being the stronger direction) shows a 2040% higher tensile modulus than 90 direction. The tensile strength of NMT materials is lower than the GMT, but it is increased with increased bre content and it is expected to improve further if coupling agents are used. Even the tensile stress is strongly dependent on the direction. For example Mhlmeier NMT showed a tensile strength of about 57 MPa in 0 direction and only 31 MPa in 90 direction. Generally the NMT composites showed lower Izod impact strength compared to GMT composites in both notched and unnotched samples except Danax which showed impact properties comparable to GMT especially in 0 direction. According to the material manufacturer this is because of the high bre length. Impact, tensile properties and the microscopy study indicated that there is poor bre/matrix adhesion in all NMT composites. These results show that NMT composites have a potential to be used instead of conventional GMT in engineering applications where low weight, easily recyclable and environmental friendly materials are desirable. The NMT materials showed in most cases somewhat lower prices compared to GMT but the material suppliers count on even lower prices in the future. Acknowledgements The author would like to thank Symalit AG, Switzerland, Molybon Agentur AB, Sweden, Danax AS, Denmark and Lear Corporation, Sweden, Interior Systems AB, Tanum, for supplied materials. References
1. 2. 3. Flster, T. and Michaeli, W., Flax a Renewable Source of Reinforcing Fibre for Plastics, Kunststoffe German Plastics 83(9), 1993, 687691. Mieck, K.-P., Nechwatal, A., and Knobelsdorf, C., Potential Applications of Natural Fibre in Composite Materials, Internat. Textile Reports 75(11), 1994, 892898. Mieck, K.-P., Ltzkendorf, R., and Reussmann, T., Needle-Punched Hybrid Nonwovens of Flax and PP Fibres Textile Semiproducts for Manufacturing of Fibre Composites, Polymer Comp. 17(6), 1996, 873878. Heijenrath, R. and Peijs, T., Natural-Fibre-Mat-Reinforced Thermoplastic Composites Based on Flax Fibres and Polypropylene, Adv. Comp. Letter 5(3), 1996, 8185. Hornsby, P. R., Hinrichen, E., and Taverdi, K., Preparation and Properties of Polypropylene Composites Reinforced with Wheat and Flax Straw Fibres, J. Mater. Sci. 32(4), 1997, 1009 1015. Sanadi, A. R., Cauldeld, D. F., and Rowell, R. M., Reinforcing Polypropylene with Natural Fibres, Plastic Engin. 4, 1994, 2728. Oksman, K. and Lindberg, H., Interaction between Wood and Synthetic Polymers, Holzforschung 49, 1995, 249254. Oksman, K., Improved Interaction between Wood and Synthetic Polymers in Wood/Polymer Composites, Wood Sci. Technol. 30, 1996, 197205. Bledzki, A. K., Reihmane, S., and Gassan, J., Properties and Modication Methods for Vegetable Fibers for Natural Fiber Composites, J. Appl. Polymer Sci. 59, 1996, 13291336.

4. 5.

6. 7. 8. 9.