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Polypropylene Composites with Natural Fibers and Wood - General Mechanical Property Profiles Lukas Sobczak, Reinhold W. Lang, Andreas Haider PII: DOI: Reference: To appear in: Received Date: Accepted Date: S0266-3538(11)00448-9 10.1016/j.compscitech.2011.12.013 CSTE 5140 Composites Science and Technology 24 October 2011 16 December 2011

Please cite this article as: Sobczak, L., Lang, R.W., Haider, A., Polypropylene Composites with Natural Fibers and Wood - General Mechanical Property Profiles, Composites Science and Technology (2012), doi: 10.1016/ j.compscitech.2011.12.013

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Polypropylene Composites with Natural Fibers and Wood General Mechanical Property Profiles

Polypropylene Composites with Natural Fibers and Wood - General Mechanical Property Profiles
Lukas Sobczaka1, Reinhold W. Langb, Andreas Haidera
Competence Centre for Wood Composites and Wood Chemistry (Wood K plus), Division WoodPolymer-Composites; St. Peter-Strae 25, 4020 Linz, Austria Johannes Kepler University Linz, Institute for Polymer Materials and Testing; Altenberger Strae 69, 4040 Linz, Austria
1 b a

Corresponding Author l.sobczak@klus-wood.at Tel.: +43 732 6911 4082 Fax: +43 732 6911 2864

Abstract
Natural Fiber Composites (NFC) and Wood Polymer Composites (WPC) based on polypropylene (PP) have gained increasing interest over the past two decades, both in the scientific community and in industry. Meanwhile, a large number of publications is available, but yet the actual market penetration of such materials is rather limited. To close the existing gap between scientific and technical knowledge, on the one hand, and actual market applications, on the other, it is the purpose of this paper to analyze the current state of knowledge on mechanical performance profiles of injection molded NFCs and WPCs. As the composite properties are a result of the constituent properties and their interactions, special attention is also given to mechanical fiber/filler properties. Moreover, considering that NFCs and WPCs for a variety of potential applications compete with mineral reinforced (mr; represented in this study by talc), short glass fiber (sgf), long glass fiber (lgf) and short carbon fiber (scf) reinforced PP, property profiles of the latter materials are included in the analysis. To visualize the performance characteristics of the various materials in a comparative manner, the data were compiled and illustrated in so-called Ashby plots. page 1 of 22

Polypropylene Composites with Natural Fibers and Wood General Mechanical Property Profiles

Based on these comparisons, an assessment of the substitution potential of NFCs and WPCs is finally performed, along with a discussion of still open issues, which may help in guiding future material development and market application efforts. Keywords: Natural Fiber Composites (NFCs), Wood (A), Short-fiber composites (A), Mechanical properties (B), Injection molding (E)
Abbreviation NFC WPC Mw IS m% mr sgf lgf scf PP-(x%)y unbl., bl. u.K.p., bl.K.p. Ten. Explanation Natural Fiber Composite, meaning a fiber/matrix composite that contains natural fibers or wood based cellulose fibers Wood Polymer Composite, meaning a filler/matrix composite that contains wood particles Weight average molecular mass Impact strength mass percent mineral reinforced short glass fiber, usually below 1 mm in length long glass fiber, usually 5 10 mm in length short carbon fiber Polypropylene reinforced with y (x m% of y) bleached, unbleached (Figure 4-1, Figure 4-2, Figure 4-3) unbleached Kraft pulp, bleached Kraft pulp (Table 4-1) Tencel, wood based cellulose fiber (Table 4-1)

Table 0-1: Abbreviations used in the text;

Introduction

While polyolefins, in particular PP, have been reinforced commercially with glass fibers and particle minerals (e.g. talc, wollastonite) for several decades, more recently natural fibers and wood have become of engineering and commercial interest to produce novel classes of natural fiber composites (NFC; see Table 0-1 for abbreviations) and wood polymer composites (WPC) [1-3]. In terms of markets and applications, it is particularly the automotive industry [4-6] and the building and construction industry [7-9] which have expressed interest in using such materials. Along with cost saving aspects and expected ecological benefits (e.g. improvement in CO2-balance [10, part III;11;12]), the main motivation driving these developments is related to the mechanical property profiles of natural fibers and wood, which indicate a substantial reinforcement potential. Combined with the low density of natural fibers page 2 of 22

Polypropylene Composites with Natural Fibers and Wood General Mechanical Property Profiles

and wood (see Table 2-1), NFCs and WPCs may result in lighter weight structures when compared to mineral reinforced (mr), short glass fiber (sgf), long glass fiber (lgf) and short carbon fiber (scf) reinforced materials [13-15]. In addition, NFCs and WPCs can be processed similar to these other material classes, e.g. by injection molding and extrusion. In fact, in terms of processing behavior, NFCs and WPCs may even offer advantages with regard to equipment wear [13;15;16]. Despite the high industrial interest in NFCs and WPCs, and the significant scientific efforts particularly over the past decade, no comprehensive overview exists on mechanical property profiles of various material grades that allows for a proper comparison among these novel PP-based materials. Such a comparison is also lacking with materials already used commercially, such as mr, sgf, lgf and the more novel scf composites, with which NFCs and WPCs are supposed to compete. Hence, the overall objective of this paper is to provide a comprehensive overview of the mechanical property profiles of NFCs and WPCs, and to compare these properties to those achieved by existing commercial composites based on mineral, glass and carbon fiber reinforcements. For various reasons (cost and/or performance), NFCs and WPCs are frequently produced with high fiber/wood content, so that special emphasis was paid to cover the natural fiber or wood content range up to about 70 m%. This reinforcement level also corresponds to the limit of adequate processability of high quality products by injection molding [17].

Materials and Methods

All of the data presented here is taken from scientific literature or from material data sheets provided by the suppliers. To ensure a sufficient comparability of the material

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property values given, only data generated utilizing injection molded specimens and applying equivalent test procedures and conditions has been included. Table 2-1 provides some general information on the densities and current prices for the constituents of the various material grades included in this overview. Throughout this paper, the term natural fibers refers to plant-based fibers (like jute, hemp, kenaf, sisal, flax) and wood based cellulose fibers (Kraft pulp, unbleached cellulose, regenerate cellulose such as Tencel). On the other hand, the term wood particles as they are used in WPCs refers to the grinded state of solid wood which lacks the characteristic of a higher aspect ratio. One advantage of natural fibers clearly apparent from Table 2-1 is their lower density. While conventional reinforcements (scf, sgf, talc) exhibit a density range from 1.7 to 2.8 g/cm3, the density range for natural fibers and wood (compressed state as it occurs in WPCs as a result of processing) is from about 1.3 to 1.6 g/cm3. The effects of the processing steps from solid wood to wood particles, and of compression during WPC processing, are expected to result in a corresponding alteration in mechanical properties. Since no data for modulus and strength of wood fillers in the compressed state are available, the comparisons performed in chapter 3 with regard to wood as reinforcement are perhaps of limited quantitative value but were nevertheless included to provide an overall relative picture. The reinforcement prices range from about 0.2 /kg for spruce at the lower end to 20.0 /kg for short carbon fibers at the upper end. For comparison, polypropylene typically has a price level of 1.0 to 1.4 /kg, depending on the specific grade and the order volume. In other words, from the reinforcements considered in this overview,

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most are below the price level of the PP matrix, while in some cases, the reinforcement prices may exceed the PP matrix price.
Material PP scf sgf Talc Tencel Flax Hemp Jute Kenaf Sisal Spruce Density [g/cm3] 0.90 1.70 1.77 2.50 2.75 1.55 1.50 1.48 1.30 1.45 0.45- 0.50 (uncompr.) ~ 1.30 (compressed) Price [ /kg] 1.0 1.4 10.0 20.0 0.9 1.6 0.3 1.0 0.3 1.3 (upper bound: pellets) 0.3 1.0 (upper bound: pellets) 0.5 0.7 0.4 1.5 0.5 0.8 0.2 - 0.4 Source [18] [13;19;20] [13;21] [22] [23] [13;24, page 12] [25, page 119;26] [14;25, page 119;26] [13;25, page 119] [14;27] [13;25, page 119;27] [28;29]

Table 2-1: Densities and prices of Polypropylene and several conventional reinforcements plus natural fibers and wood (spruce);

For the material property data of the reinforcement constituents and the respective PP compounds processed by injection molding (sections 3 and 4, respectively), the Ashby plot [30] was chosen as means of presentation. In terms of relevant properties, Ashby plots were generated as tensile strength vs. tensile modulus for the reinforcement constituents, and as tensile strength vs. tensile modulus and impact strength vs. tensile modulus for PP and its various compounds (i.e., PP composites). Due to the lack of data covering a wider range of test conditions, for IS values room temperature data for unnotched Charpy specimens were selected. To allow for a comparison of the material property profiles in terms of the potential for lightweight structural design, the Ashby plots for tensile modulus and strength are illustrated for absolute property values but also for specific property values (i.e. absolute values divided by the respective material density). For the latter representations, the proper material density values were obtained from the literature when available, or were page 5 of 22

Polypropylene Composites with Natural Fibers and Wood General Mechanical Property Profiles

calculated applying a simple rule-of-mixture model from the constituent volume contents and the constituent densities in Table 2-1.

Fiber properties

The tensile strength vs. modulus properties of various natural fibers are compared to those of conventional fibers for PP reinforcement (sgf/lgf, scf) in Figure 3-1 and Figure 3-2 in terms of absolute properties and specific properties, respectively. The data for the various fiber types and grades were taken from the references indicated in Table 3-1 and, in the case of the natural fibers, represent dry fiber conditions. Before depicting the fiber properties in Ashby-plots, the following aspect with regard to the variability of fiber strength and modulus values must be pointed out. While strength and modulus of specific grades of conventional fibers usually meet quite narrow tolerances, natural fibers are known to vary substantially [13;31]. For example, modulus and strength values of jute fibers may vary from about 13 - 27 GPa and from about 390 - 770 MPa, respectively. Similar variations are known for wood (e.g., European spruce: Youngs modulus range from about 7 - 21 GPa; tensile strength range from 20 - 250 MPa [28]). Kenaf has not yet been investigated to an extent so that similar variations could be deduced from the literature. In any case, the reported variability of properties of a specific natural fiber type is accounted for by including the reported upper and lower bound values in the Ashby plots below. In terms of absolute properties, Youngs modulus values of natural fibers and wood range from about 7 - 70 GPa [14;28], while modulus values for conventional fibers range from about 70 GPa (sgf/lgf [13]) to 240 GPa (scf [19]). Alternatively, the conventional fibers exhibit significantly higher strength values, ranging from about 2,000 MPa (E-type sgf/lgf [13]) to 4,000 4,570 MPa (scf, S-type sgf/lgf [13]), page 6 of 22

Polypropylene Composites with Natural Fibers and Wood General Mechanical Property Profiles

compared to natural fibers and wood ranging from about 20 - 1,100 MPa [13;28]. In other words, conventional fibers significantly outperform natural fibers and wood in terms of strength, but in terms of modulus, some natural fibers such as hemp and kenaf nearly reach the values of at least glass fibers. Of course, when comparing just the two groups of natural reinforcements in Figure 3-1, the fiber reinforcements are seen to supersede the wood reinforcements both in terms of strength and modulus. Due to the density differences of the various fiber types and wood, the specific properties depicted in Figure 3-2 are somewhat different to those in Figure 3-1. First, as described above (section 2), the data points for the wood type reinforcements are of limited relevance for PP composites, as they correspond to an uncompressed state with very low density which is not representative of the more highly compressed state in a PP compound. Second, the specific modulus data for glass fibers are shifted into the range of the corresponding values of natural fibers, with hemp even exceeding the specific modulus values of glass fibers. Third, the highest values for specific strength of natural fibers are achieved for flax, which is now approaching the lower end of the specific strength range for glass fibers. Finally, carbon fibers, due to their low density, still retain their superiority compared to all other fibers with regard to specific modulus values. The lower density compared to glass fibers now also translates into higher values for specific strength of the carbon fibers.
Carbon [13;19] Glass [13] Tencel [23] Flax [13;31] Hemp [14;31] Jute [13] Kenaf [14] Sisal [13] Spruce [28] Oak [32]

Table 3-1: References for the tensile property data of the various reinforcement types presented in Figure 3-1 and Figure 3-2.

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5000 4500
Specific Tensile Strength [kJ/kg]

2500

4000 3500

2000

Tensile Strength [MPa]

3000 2500 2000 1500 1000 500 European Spruce 0 0 50 100 150 200 250 Young's Modulus [GPa] European Oak Tencel Hemp Kenaf Carbon E-glass S-glass Flax Jute Sisal

1500 Carbon 1000 Tencel 500 Hemp E-glass S-glass Flax Jute Sisal European Spruce 0 50 100 European Oak 150

Specific Young's Modulus [MJ/kg]

Figure 3-1: Ashby plot presenting the absolute tensile strength versus the Youngs modulus for various fiber types.

Figure 3-2:

Ashby plot presenting the specific tensile strength versus the specific Youngs modulus for various fiber types (property divided by density).

Composite properties

4.1 Tensile properties

The tensile properties of various PP composites are depicted in Figure 4-1 and Figure 4-2 in absolute and relative terms, respectively, as strength vs. modulus diagrams. The data for the various materials were taken from the references indicated in Table 4-1 and, in the case of the natural fiber/filler composites, represent dry specimen conditions. In both diagrams, the property range covered by neat PP homopolymers is included for comparison. From the illustration of the absolute properties in Figure 4-1 it becomes apparent that the property regions covered by conventional fiber/filler composites and by the natural fiber/filler composites approach one another, although they are clearly separated in Figure 3-1, which depicts the absolute fiber/filler properties. While the general tendency of this shift can be explained by rule of mixture considerations, several effects remain remarkable. To begin with, the property areas covered by the NFCs and the WPCs overlap to a greater extent than is the case just for the page 8 of 22

Polypropylene Composites with Natural Fibers and Wood General Mechanical Property Profiles

reinforcement constituents in Figure 3-1. This is at least partly due to the fact that the WPCs included contain up to 70 m% wood particles while the NFCs are limited to a fiber content of about 60 m% (in terms of fiber/filler volume content the differences are slightly larger due to differences in density; see Table 2-1). Nevertheless, while with WPCs modulus/strength combinations of up to about 7 GPa / 55 MPa [17;33] are obtained, for NFCs about 11 GPa / 75 MPa may be achieved [34]. When comparing the natural fiber/filler composite data to conventional PP composite data, the following observations are made. NFCs and WPCs exist that outperform PP-talc composites, which exhibit modulus/strength values of about 4 GPa / 35 MPa [35], both in terms of modulus and tensile strength. Conversely, PP-sgf/lgf composites cover a modulus/strength regime from about 5 GPa / 75 MPa [36] up to 13 GPa / 135 MPa [37], which is clearly above the property range covered by NFCs and WPCs. Interestingly, the values achieved for PP-scf composites, both in scientific investigations [19] and for commercial products [38;39], fall significantly short of rule of mixture based expectations. This is particularly the case for the tensile strength values, where PP-scf composites cover a range similar to NFCs and even overlap with WPCs. Merely, the modulus values of PP-scf composites exceed those of the other material classes in Figure 4-1, although in this case too, to a lesser degree than expected based on the respective fiber modulus data.

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150 140 130 120 110 100
Tensile Strength [MPa]

neat PP Carbon 20 27 40 Glass 20 sgf 30 sgf 40 sgf 50 lgf Talc 20 40 Flax 25 30 60 40 Hemp

120

neat PP Carbon 20 27 40 Glass 20 sgf 30 sgf 40 sgf 50 lgf Talc 20 40 Flax 25 30 60 40 Hemp Jute 40 50 60 Kenaf 20 40 50 60 30 Sisal unbl. Kraft pulp 30 45 40 bl. Kraft pulp

110

100

90

80
Specific Tensile Strength [kJ/kg]

90 80 70 60 50 40 30 20 10 0 0 2 4 6 8 10 12 14 16 18 20 Young's Modulus [GPa]

70

Jute 40 50 60 Kenaf 20 40 50 60 30 Sisal unbl. Kraft pulp 30 45 40 bl. Kraft pulp 33 Tencel Wood particles 30 40 50 60 70 22 24

60

50

40

30

20

33 Tencel Wood particles 30 40 50 60 70 0 2 4 6 8 10 12 14 16 18 20 22 24

10

0 Specific Young's Modulus [MJ/kg]

Figure 4-1:

Ashby plot presenting the tensile strength versus the Youngs modulus of various PP compounds. The numbers in the legend give the fiber/filler content in [m%]. Content [m%] 20 27 40 20 30 40 50 20 40 Sources [39] [19] [19;38] [36] [50;51] [35] [37] [57;58] [35;60] Filler Flax Hemp Jute Kenaf

Figure 4-2:

Ashby plot presenting tensile strength versus Youngs modulus of compounds (property density). Filler u.K.p. b.K.p. Ten. Wood Content [m%] 30 45 40 33 30 40 50 60 70

the specific the specific various PP divided by Sources [41] [41] [47] [23] [52;53] [53;55;56] [17;33;53] [17;33] [17;33]

Filler scf sgf lgf Talc

Sisal

Content [m%] 25 30 60 40 40 50 60 20 40 50 60 30

Sources [40] [42-45] [46] [47-49] [34] [34;54] [34] [59] [59;61] [35;61] [59] [62;63]

Table 4-1: References for the mechanical property data of the various compounds presented in Figure 4-1, Figure 4-2 and Figure 4-3; neat PP data is taken from [64;65].

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The specific modulus/strength diagram in Figure 4-2 reveals similar tendencies as discussed above for the absolute property ranges of the various material types. Reflecting the density differences, the NFCs and WPCs now appear further improved compared to PP/talc composites, and the upper bound strength ratio between PP/lgf and NFCs is now reduced from about 1.8:1 in terms of absolute strength to 1.5:1 in terms of specific strength. In terms of specific modulus, the upper bound values of these two material classes now even approach one another. Similar ratios were found by Wambua et al. in a comparison of glass fiber and natural fiber reinforced PP composites (i.e. 40 m% fiber content, prepared by a film stacking method) [66]. Furthermore, the differences in the upper bound values of specific modulus data between PP-scf and PP-sgf are slightly enhanced.

4.2 Impact properties

The impact properties of the various material classes are illustrated and compared in Figure 4-3 as unnotched Charpy values vs. Youngs modulus values. Most remarkably is the specific NFC grade utilizing the commercial cellulose fiber Tencel. It is the only reinforcement type that allows for significant improvements in modulus without sacrificing the impact properties when compared to the lower bound range of neat PP which represents grades with low weight average molecular mass, (Mw) [23]. However, higher Mw PPs reach unnotched Charpy impact strength (IS) values reaching 100 kJ/m2 and even higher, up to a point where unnotched specimens do no longer break upon the impact [67]. Apart from the Tencel reinforced PPs, unnotched impact strength values of all other PP composites are reduced compared to neat PP, with PP-sgf exhibiting the least reductions, followed by PP-talc composites and NFCs, with WPCs revealing the most significant reductions. A study by Wambua et al. on compression molded composites prepared by a film stacking page 11 of 22

Polypropylene Composites with Natural Fibers and Wood General Mechanical Property Profiles

method (cited already above for tensile properties) also supports the data reviewed here for injection molded composites in terms of material ranking and property ratios. Thus, for a comparable fiber content, glass mat reinforced PPs also exhibit about twice the unnotched Charpy IS of natural fiber mat reinforced PPs [66]. Numerous studies exist on factors controlling the impact strength of NFCs and WPCs. As to the influence of the particle size, it is clear that this parameter may play an important role, however no clear and unambiguous tendencies can be deducted from the published literature as yet [52;68-71]. Conversely, for unnotched specimens, IS is usually improved by enhanced coupling [45;55;71;72], whereas for notched specimens, the improvement is often not so significant, with even reductions in impact values resulting from increased coupling having been reported [56;68;73-77]. Furthermore, it is well proven that IS of NFCs and WPCs can be enhanced significantly by rubber toughening of the PP matrix, however in all cases at the cost of modulus reductions [55;78-80]. Nevertheless, despite all the efforts to study impact properties of NFCs and WPCs, no study is available that unambiguously explains the cause of the poor impact performance of these materials, when compared to neat PP and PP-sgf and PP-talc composites. Moreover, there is not a sufficient database for a comprehensive comparison of impact properties for the material grades of interest to this paper. Particularly, a more detailed analysis of the effects of notches on impact strength and the influence of test temperature, to deduce brittle-ductile transitions, is lacking. In this context, it is known from preliminary investigations that notched impact properties of PP-sgf composites and PP composites with Tencel fibers may even exceed the values obtained with neat PP [23;36;50;51]. Clearly, more work is needed to study and perhaps optimize the impact behavior of NFCs and WPCs. page 12 of 22

Polypropylene Composites with Natural Fibers and Wood General Mechanical Property Profiles
60 neat PP
Glass 20 sgf 30 sgf

IS Charpy unnotched [kJ/m2]

50

40

Talc 20 40 30 Flax

Figure 4-3: Ashby plot presenting the unnotched Charpy impact strength vs. the Youngs modulus of various PP compounds. The numbers in the legend give the fiber/filler content in [m%].

30

unbl. Kraft pulp 30 45 33 Tencel Wood particles 30 40 50 60 70 0 2 4 6 8 10

20

10

0 Young's Modulus [GPa]

Open Issues

As modern PP-NFCs and PP-WPCs still represent rather novel classes of materials, and despite the fact that quite a lot is known on the properties and on the behavior of these materials, it is also not surprising that there are a number of issues that are as yet unresolved and thus deserve further attention. These open issues include aspects related to material property and performance profiles, to the processing behavior and adequate processing conditions, and last but not least aspects in relation to the ecological impact and life cycle assessment. With regard to material and performance related issues, a particular problem in the case of polyolefin-based NFCs and WPCs is the inherent incompatibility between the non-polar hydrocarbon matrix and the usually hydrophilic ligno-cellulosic

reinforcements. While numerous scientific studies in recent years aimed at improving the interfacial adhesion in these materials, a detailed understanding of the mechanisms of bonding affecting and improving the fracture properties and the failure behavior is still lacking [14;81-84].

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Another aspect of practical relevance that needs further study is related to the effects of moisture on the material properties and performance profiles of polyolefinic NFCs and WPCs. For example, for WPCs with high filler levels (70 87 m%), Svoboda [10, page 145 ff.] found that the tensile properties (strength and modulus) are reduced by up to 55 % (70 m% wood) when the material has absorbed more than 10 % moisture upon water immersion. Viksne et al. report significant reductions (up to 30%) in flexural properties for PP-based WPCs with 50 m% filler content upon three water absorption/desorption cycles [85]. Similar effects on tensile properties were found by Arbelaiz et al. [46] for PP reinforced with 20 60 m% flax fibers. These studies provide a good indication of the property reductions to be expected by moisture absorption, and numerous other reports on the effects of moisture on the mechanical behavior exist [71;86-100]. And yet, considering the pronounced sensitivity to moisture uptake of these PP based NFCs and WPCs, further investigations are needed to deduce guidelines for component design and performance for applications under typical climatic conditions. Other aspects not sufficiently addressed so far are related to expected improvements in noise and vibration damping of PP based NFCs and WPCs [6;101-103]. In this context, advantages of NFCs and WPCs over conventional polymer composites are frequently argued, however, quantitative data and information is rather scarce. Thus, to our knowledge no article exists which compares the acoustic properties of, for instance, NFC or WPC based automotive interior panels with PP-talc based panels. On the other hand, NFCs and WPCs are used in several applications with proven positive results in terms of acoustic performance (e.g. automotive interior [101], musical instruments [104] loudspeaker-boxes etc. [105]).

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As has been addressed above, and completing the list of open issues related to NFC and WPC properties, natural fibers and wood are known to exhibit substantial lot-tolot variations in their properties depending on plant growth and harvesting conditions [12;106, page 8]. Moreover, although several studies exist [107-111], emission and odor problems that may potentially arise particularly in indoor building and automotive interior applications deserve further attention and investigations. Turning to open issues related to processing behavior and conditions of NFCs and WPCs, reduced equipment wear is often argued to be advantageous compared to PP-sgf/lgf or PP-mr [13;15;16]. While it seems likely that natural fibers or wood, containing mostly cellulose and lignin, should cause less abrasion on the surfaces of processing equipment than hard and sharp-edged glass fibers, for example, no published study exists supporting and quantifying this assertion. In addition, more precise pre-conditioning and processing conditions need to be defined to account for the hydrophilicity of natural fibers/fillers, and for the degradation sensitivity of NFC or WPC compounds when being processed at elevated temperatures under simultaneous mechanical shear [112-114]. Another processing-related problem that arises when natural fibers are used as reinforcements is their inaptitude to metering via usual dosing scales. Traditionally, such fibers are supplied as bales or staple fibers, and are thus not free flowing. Basically, there are two ways to overcome this drawback: First, by cutting or milling the fibers down, until a sufficient ease of flow is achieved. Second, pelletizing of the fibers is an option. Both of those technical solutions increase costs. Furthermore, the first approach potentially leads to a reduction of composite properties by a reduced fiber length. The second approach, on the other hand, raises the issue of redispersion of the fibers during the compounding step and poses a problem when the page 15 of 22

Polypropylene Composites with Natural Fibers and Wood General Mechanical Property Profiles

pellets are well consolidated. A method which avoids those issues is the long fiber granulate (LFG) process developed by the Thuringian Institute of Textile and Plastics Research (TITK) [115]. It is a pull-drill treatment by which strands of fibers are coated with a thermoplastic matrix. Thus, granules containing long fibers (of the length of the granule) can be produced. Despite appearing like a promising alternative, to our knowledge the process has not yet been implemented on industrial scale. There are several other topics and problems that require attention when applying NFCs and WPCs in technical products. These include the long-term performance of these materials and products, both in terms of mechanical properties but also concerning visual appearance (e.g. color change). In fact, quite a few studies are available on specific effects of weathering on optical and mechanical properties, and thus on the long-term stability of these materials. The most obvious consequence of weathering on WPCs is whitening resulting from lignin degradation [116-120]. Of course, weathering also affects mechanical properties, usually leading to significant reductions [93;116;121;122]. However, analogous to the effect of moisture absorption, it is difficult here too to provide general guidelines for component design and performance for applications under typical long-term weathering conditions. To complete the most important requirements as to material properties and product performance profiles, flame retardance is a prime prerequisite in certain applications. As PP-based NFCs and WPCs per se are not improved over neat PP and in certain properties are even inferior [123;124], large amounts (usually 10 30 m%) of flame retardant additives must be employed to achieve significant improvements [125-127]. Of course, utilizing such high amounts of additives may have pronounced effects on the processing behavior and the remaining property profile of these materials [124;128;129], which must be accounted for in specific applications. page 16 of 22

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Finally, and despite the fact that ecological considerations are frequently used as selling argument [7;130], only limited information is available on validated ecobalances and life cycle assessment (LCA) data of PP based NFCs and WPCs. Svoboda provides a performance oriented assessment comparing several materials based on renewable resources, including wood and highly filled WPCs, and conventional materials like PE, PP, PVC and aluminum, among others [10, page 177 ff.]. Depending on the conditions applied, WPCs may or may not be favorable in terms of ecological performance. Furthermore, Michaud et al. performed LCA studies on highly filled PE-based WPCs [131]. Also, hardly any LCA data exist on NFCs, and the available data as to the actual ecological performance are ambiguous [11;132;133]. Hence, as for the other issues mentioned above, further studies are needed to unambiguously provide information on the ecological performance of particularly polyolefin and PP based NFCs ad WPCs compared to other materials.

Summary and Conclusions

As to the fiber properties, conventional fibers such as short/long glass fibers (sgf/lgf) and short carbon fibers (scf) exhibit significantly higher strength values than even the best natural fibers (factor 2 4). In terms of modulus, some natural fibers, like, e.g., hemp and kenaf, show values similar to sgf/lgf, with scf modulus values superseding these fibers by a factor of 3. Due to the lower density of natural fibers compared to glass fibers, the specific properties of natural fibers, on the one hand, and sgf/lgf, on the other, shift closer together. Particularly remarkable is that hemp even supersedes sgf/lgf in the specific modulus, and flax approaches sgf in specific strength. For the resulting PP composites, in terms of absolute properties, the picture is largely similar, with some remarkable exceptions. First, the relative difference between NFCs page 17 of 22

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and WPCs, on the one hand, and PP-sgf/lgf on the other, is reduced due to rule of mixture based effects. Second, WPCs supersede PP-talc composites, both in modulus and strength, while NFCs largely overlap with the PP-sgf/lgf range for modulus and approach its lower end for strength. In terms of specific properties the position of NFCs and WPCs relative to the conventional composites (except for PPscf) is again somewhat improved, due to the aforementioned density differences. The perhaps most significant drawback of NFCs and WPCs, compared to the conventional PP composites, is related to their lower IS. While NFCs at least partly overlap with the PP-talc range, all WPCs exhibit inferior impact behavior. It should be pointed out, however, that one NFC grade, i.e. PP-Tencel, performs remarkably well, being the only PP composite presented which retains the (unnotched Charpy) IS level of neat PP, thus even exceeding PP-sgf composites. Overall, NFCs may substitute PP-sgf composites when some reduction in strength is accepted. WPCs, on the other hand, may replace PP-talc composites, in applications where impact strength is not critical. Reflecting on the current state of knowledge and technology in the field of NFCs and WPCs, there are several open issues and aspects yet to be addressed, These include the effects of temperature and moisture uptake on mechanical properties and processing behavior. Moreover, there is a large variability in properties of natural fibers and wood, depending on growth and harvesting conditions. Also, for a number of advantages usually associated with NFCs and WPCs (i.e. reduced abrasiveness in processing, improved noise damping behavior, improved overall ecobalance compared to conventional composites) there is a need for quantitative and reliable data in support of these reputed benefits. Finally, based on constituent property considerations, the performance potential of natural fiber and wood composites at this stage may not yet be fully exploited. Hence, page 18 of 22

Polypropylene Composites with Natural Fibers and Wood General Mechanical Property Profiles

further research is warranted on elucidating structure-property relationships for these materials to overcome current weaknesses (e.g. impact strength).

7
[1] [2] [3] [4] [5] [6] [7] [8] [9] [10] [11] [12] [13] [14] [15] [16] [17] [18] [19] [20] [21] [22] [23] [24] [25] [26] [27] [28] [29] [30] [31] [32] [33] [34] [35] [36] [37] [38] [39] [40] [41] [42] [43]

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