Paper No: MBSK 02-205____________ An ASAE/CSAE Meeting Presentation

Engineering Properties of Flax Fiber and Flax Fiber-Reinforced thermoplastic in Rotational molding
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T. Powell , S. Panigrahi , J. Ward , L. G. Tabil , W. J. Crerar , S. Sokansanj

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Department of Agricultural and Bioresource Engineering, University of Saskatchewan, 57 Campus Drive, Saskatoon, SK. S7N 5A9

Environmental Sciences Division, Oak Ridge National Laboratory, One Betchel Valley Road, Bldg 1059, P.O. Box 2008, Oak Ridge, TN 37831-6422USA

Written for presentation at the 2002 ASAE/CSAE North-Central Intersectional Meeting Sponsored by ASAE and CSAE Parktown Hotel Saskatoon, Saskatchewan, CANADA September 27-28, 2002

Summary:
The objective of this study is to determine the physical properties of flax fiber, as well as flax fiber-reinforced LLDPE and HDPE, in order to develop optimal manufacturing parameters for rotational molding of composites. Some of the parameters investigated include tension tests for yield strength, impact tests to determine allowable impact loads, and thermal properties of both the flax and the LLDPE matrix. The tension and impact testing was performed on manufactured samples of varying fiber contents, and the resulting relationship between performance and fiber percentage was analyzed. Also, since the rotational molding method is greatly dependant on temperature, several thermal properties such as thermal conductivity, thermogravimetric profiles and specific heat of the flax fiber and matrix were analyzed. Tension testing was performed using an instron load cell, and the resulting relationships were analyzed, with special interest in fiber content. The falling weight impact tests were performed in order to get a more solid understanding of the material behavior to impact loads. Most detrimental to consistency, however, is the thermal properties of the composite materials. Various heating and cooling rates of the material, as well as oven time and rotational speed all affect the finished product.

Keywords: Flax fiber, rotational molding, plastic composites, engineering properties, thermal conductivity, tensile test

Engineering Properties of Flax Fiber and Flax Fiber-Reinforced thermoplastic in Rotational molding
1 1 1 1 1 2

T. Powell , S. Panigrahi , J. Ward , L. G. Tabil , W. J. Crerar , S. Sokansanj

Introduction Flax fiber presents an ecologically sound alternative to reinforcing fibers in plastic composites. Flax fibers are less dense then glass fibers, are renewable and combustible, and relatively low in price. The strength and toughness of flax fiber is comparable to that of glass fibers, and flax fiber in Saskatchewan is generally considered a waste product. In order to successfully utilize a material for industrial applications, it is first imperative to determine material properties which will affect performance. Material behavior under certain given conditions must be analyzed thoroughly in order to simulate manufacturing conditions as closely as possible. Close inspection of the rotational molding process shows that thermal stresses on the material are present, as heat is required to liquefy the matrix and mix in the filler. Heating and cooling rates are also fundamental when trying to ensure a reproducible product with adequate material performance. Slow cooling rates tend to cause crystallization within the matrix, which sacrifices material performance. A faster cooling rate is preferred since it causes favorable cohesion inside the matrix, producing a more stable product. For the scope of this paper, flax fiber was examined closely in order to determine the physical properties associated with it. Also, several manufactured parts were tested in order to get a good understanding of the effects that different fill ratios and matrix type have on material performance. Testing on manufactured parts included instron tension tests, dart impact tests, and some thermogravimetric analyses. A digital thermal conductivity probe was also employed to determine some thermal properties of a pure matrix sample, as well as pure flax fiber and fiber-straw mixture. Materials and Methods Thermogravimetric Analysis Thermogravimetric analysis of flax fiber, flax straw, and pure matrix were conducted at a heating rate of 20 degrees per minute, with a gas flush rate of 30 ml per second. Sample sizes were generally taken as 3.2-4.2 mg, and each sample type was analyzed three times to obtain a representative data field. The TG weight loss data was calculated by Graphware (Mettler TG 50 Thermobalance). The primary decomposition band extended from 210220 C, and continued on until nearly 400 C. However, flax fiber contains large amounts of cellulose, hemicellulose, lignin and pectin, all of which would affect the reaction to thermal stresses differently. The fiber composition could be surmised from data pertaining to the thermal decomposition of each of its components, but this was not performed since fiber composition was not a relevant factor. Thermal Probe Analysis Thermal properties such as thermal conductivity, resistivity and diffusivity were measured from samples consisting of pure flax fiber, pure matrix and combinations of both. Samples were ground into a fine powder and compressed within a beaker to ensure that all porous air space was removed from the sample and would not interfere with heat transfer between the particles. The samples were then placed into a constant temperature bath in order to condition the sample and determine the affects of varying temperature on properties. A KD2 thermal properties analyzer probe (Decagon,Pullman, WA) was used for measurement, and was capable of measuring all three parameters from the same reading. Tension Testing An Instron SATEC Systems, Inc. Universal testing machine (Grove City, PA) was used to perform the tensile strength tests. Each sample was manufactured by way of rotational molding, and the familiar dog-bone shape was utilized in the testing procedure. Samples were of varying thickness and so therefore had to be ground into a more uniform size. Each tension test was performed with a loading rate of approximately 5 N/s, and each test was performed until tensile failure occurred. Manufactured samples included fiber fill ratios of 5%, 10% and 30% as 2

well as no fiber and cross-linked fiber. This was done in order to achieve a representation of how the fill ratio affects the material performance. Impact Testing A falling-weight drop impact test was employed in order to better understand the impact properties of the manufactured biocomposites. Again, the fill ratio was varied to see the effect that the fibers had on material performance. Falling weight impact testing is more or less a comparative method of analysis. A charpy impact tester (Tinius Olson Testing Machine, Willowgrove, PA) was also used to give a direct reading of impact energy. Samples were cut into thin rectangular rods of varying dimensions and were then smashed with the charpy pendulum and the impact energy at failure was recorded. However, the samples used in the charpy tests were not sufficient in size to yield a reading, and so this method of data acquisition was disregarded. Results and Discussion The thermogravimetric analysis showed that pure flax fiber generally followed a degradation profile starting at approximately 200-210 C, and continued to decompose until a temperature of near 400 C was reached. This decomposition profile is typical of flax fiber, as can be seen from the cited literature (Weilage, et al). As temperatures beyond 400 C were reached, the sample disintegrated into ash, and so a constant mass was achieved. Processing temperatures of 250 C were used in the manufacturing, which was acceptable since thermal degradation was not predominant at this temperature. Also, one must consider the effect of the matrix on the heating of the mixture. Generally, pure HDPE showed degradation beginning at approximately 410-430 C. Therefore, the matrix absorbed a great amount of heat, taking the thermal stresses off of the flax fiber. Shown below are typical profiles for pure HDPE and pure flax fiber, respectively.
Mass (m g) vs. Tem p. (deg C) 110 108 106 104 Mass (mg) 102 100 98 96 94 92 90 0 100 200 300 Tem perature (deg C) Test Run pure HDPE Blank Run 400 500 600

Figure 1. Thermogravimetric profile for pure HDPE matrix

Mass (mg) vs. Temp. (deg C)

89

88.5

88

Mass (m g)

87.5

87

86.5

86

85.5 0 100 200 300 Temperature (deg C) Test Run pure fibre Blank Run 400 500 600

Figure 2. Thermogravimetric profile for pure flax fiber The thermal conductivity, resistivity and diffusivity were measured using a thermal conductivity probe. Testing was conducted using a constant temperature bath in order to determine if varying temperature would affect the values, though this proved not to be the case. Values for different sample types are shown below. Table 1. Thermal properties for selected samples Thermal sample type Temp Conductivity (C) (W/m C) pure fiber 21 0.02 30% LLDPE 22 0.05 5% HDPE 21 0.05 flax shives 22 0.04 Thermal Diffusivity (mm^2/s) 0.28 0.14 0.14 0.18 Thermal Resistivity (m C/W) 43.5 19.2 19.6 25

The above table, while only showing values taken for approximately room temperature, can be taken as constant values since the temperature variation of the water bath had no effects on the resulting data. The differences in values between the samples suggest that the natural fibers contain more air space, and thus conduct heat less efficiently, whereas the matrix samples were able to compress more completely and reduce the insulation of air pockets. Tensile testing was performed with varying levels of fill ratios in order to develop a sense of how the filling fiber affected the tensile stress. Manufactured samples containing no fiber withstood the greatest tensile forces, however, the margin between values for filled samples and pure matrix samples was very small This occurrence can be attributed to the fact that the flax fibers blended into the biocomposite disrupt the continuity of the matrix, and so therefore cause failure at forces less then maximum. Also, with the presence of the fibers, the samples tended toward brittle failure, not showing the ductility present with unaltered samples. However, the purpose of the flax fibers within the matrix is to add several favorable properties to the end product, such as cost reduction in manufacturing, and so a small sacrifice in tensile strength can be considered acceptable. Fiber orientation within the matrix also plays a significant role in material strength. When the fibers are oriented along the axis of the applied force, they are able to accept some of the load and therefore mechanical properties such as strength are enhanced. Having the fibers oriented perpendicular to the applied force is an unwanted situation, as fibers are unable to accept compressive forces, and can only add to material through the absorption of tensile forces. Shown below are some typical curves derived during tensile testing. The first set of curves represents samples tested which were only pure HDPE, whereas the next set of curves shows the behavior given from samples containing a fill ratio of ten percent flax fiber. The samples were colored during manufacturing, and numbered during the test procedures as a means of record keeping. The effect of color on tensile stress was not examined.

Red no fiber Stress Vs Strain

25 Sr s ( /m ^ ) te s N m2 20 15 10 5 0 0 0.5 strain (mm/mm) 1 red 3 red 1 red 4

Figure 3. Stress Strain relationship for pure matrix samples

re d (10% Stre ss v s. Strain )

14 12 S s (N m 2 tre s /m ^ ) 10 8 6 4 2 0 0 0.1 0.2 Strain (m m /m m ) 0.3 0.4 red (10%) 1 red (10%) 2 red (10%) 3

Figure 4. Stress Strain profile for 10% flax fiber samples Impact testing was performed using a falling weight technique to measure impact energy calculated from the potential energy of the dart mechanism. This method, however, is considered a comparative method of analysis, and does not fit itself well to graphical representation. Results for samples containing a fill ratio of ten percent and a matrix of LLDPE were most favorable, showing failure which was more ductile in nature.

Conclusion Fiber orientation affects material strength when considering tensile loading. Orientation which is parallel to the applied force produces results which are more beneficial in terms of maximum allowable load. This can be attributed to the fact that fibers cannot absorb compression, and are only structurally beneficial when placed in tension. When comparing strengths of composites filled with flax fiber to that of unaltered polymer, it appears that unaltered or pure matrix withstands greater forces before failure, but the difference in maximum tensile stresses between filled and unaltered samples was insignificant. Also, the unaltered samples were composed of high density polyethylene, whereas the filled samples consisted mainly of linear low-density polyethylene. This difference in matrix composition could explain the lower values of maximum allowable tensile stress. However, increasing the 5

fill ratio reduces the cost of production, and also enhances the materials ability to be recycled cleanly. This trade off can be viewed as acceptable when considering what applications the material is to be used for. Thermal properties of various mixtures of biocomposites were examined using a thermal probe. Varying the surrounding temperature of the samples from 5-50 degrees Celsius showed no changes in data, and so this effect can be neglected when considering heat transfer within the biocomposite. Thermogravimetric analysis showed consistent results pertaining to mass changes with respect to increasing temperature. Pure flax fiber generally followed a decomposition curve beginning at approximately 200210 degrees Celsius and ending at approximately 400 C. Samples consisting of only matrix showed a much higher tolerance for heat, with degradation beginning at approximately 410-430 C and ending at nearly 500C. Manufacturing of biocomposites took place at an oven temperature of 250 degrees Celsius, which is well within the limits of both materials. Flax fiber has a promising future in the biocomposite area, particularly that of reinforcing agents in thermoplastics. Mechanical testing showed that natural fibers perform sufficiently to be used as consumer plastics, due to the low weight, low cost of production, and adequate strength and impact resistance. Flax fiber, as a naturally occurring product, can also be easily recycled, which makes for less infringement on the environment. The testing performed for this study proves that natural fibers are able to replace other synthetic reinforcing agents in thermoplastics. Further research and development is necessary to pursue the full potential of such an abundant and overlooked resource.

References Panagrahi S., L. G. Tabil, W. J. Crerar, S. Sokansanj, 2002. Application of Saskatchewan Grown Flax Fibre in Rotational Molding of Polymer Composites, Masonville, QC: Canadian Society of Agricultural Engineering Bolton, A. J. 1994. Natural fibres for plastic reinforcement. Materials Technology 9(1/2): 12-20 Happer, C. A. 1996. Handbook of Plastics, Elastomers and Composites Stamboulis A.,, C. A. Baillie, T. Peijs 2001. Effects of environmental conditions on mechanical and physical properties of flax fibres. Composites Part A: Applied Science and Manufacturing, 32: 1105-1115. Stamboulis A., C. A. Baillie, S. K. Garkhail, T. Peijs, 2001, H. G. H. van Melick, 2000, Environmental durability of flax fibres and their composites based on polypropylene matrix. Applied Composite Materials; 7(5-6): 273-294. Weilage B., Th. Lampke, G. Marx, K. Nestler, D. Starke, 1999, Thermogravimetric and differential scanning calorimetric analysis of natural fibers and polypropylene. Thermochimica acta, 337: 169-177 Aurich T., G. Mennig, 2001, Flow-induced fiber orientation in injection molded flax fiber reinforced polypropylene. Polymer Composites, 22: 680-689. Garkhail S.K., R. W. H. Heinjenrath, T. Peijs 2000, Mechanical properties of natural-fibre-mat-reinforced thermoplastics based on flax fibres and polypropylene. Applied Composite Materials, 7(5-6) 351-372. Hornsby P.R., E. Tarverdi 1997, Preparation and properties of polypropylene composites reinforced with wheat and flax straw fibres. Journal of Materials Science, 32 (2): 443-449.