D J. Chem. Chem. Eng. 7 (2013) 626-632 DAVID PUBLISHING TENCEL®—A High-Performance Sustainable Cellulose Fiber for the Construction Industry/Composites Friedrich Suchomel* and Martin Marsche Department of New Applications, Lenzing AG, Lenzing 4860, Austria Received: April 24, 2013 / Accepted: May 14, 2013 / Published: July 25, 2013. Abstract: Fibers are used in various areas for improving the performance of different materials, commonly used are synthetic fibers and glass fibers. More and more sustainable alternatives are required to reduce energy consumption and the carbon footprint. Traditional natural fibers (like hemp or flax) very often do not fulfill requirements for construction purposes like resistance to elevated temperature or lacking purity. Also mechanical properties of natural fibers are influenced by factors like harvesting, kink bands, climate and growth conditions. Lenzing AG has put a lot of efforts into developing a sustainable fiber overcoming the above mentioned issues. The raw material for TENCEL® is wood, which is transformed into a fiber of pure cellulose in an economy friendly process as been proven by a life cycle assessment. The properties of a composite material are highly dependent on parameters like mechanical fiber properties, fiber diameter, quality of fiber dispersion and fiber matrix adhesion. Keeping these properties constant throughout the whole composite part is the factor to success. The diameter as well as the mechanical properties of TENCEL® fibers is kept within a very narrow range thanks to the unique manufacturing process. It was shown that the fiber dispersion of TENCEL® as well as the fiber matrix adhesion is better than for natural fibers. Key words: TENCEL®, cellulosic fiber, plastic reinforcement, concrete, sustainability. 1. Introduction Fibers have been used in composite materials already for centuries as technological needs demand fibers for reinforcement and improvement of various construction materials. In recent times these composite materials are tailored to the specific needs, thus a wide range of fibers are used in modern materials. Typical examples for fibers in reinforced plastic materials are glass fibers, whereas for construction material like as plaster or concrete synthetic fibers are widely used [1-3]. More and more sustainable materials are required to reduce energy consumption and the carbon footprint. Although there is a widespread interest in natural fibers like hemp or flax for manufacturing composite materials, these natural fibers often do not fulfill the requirements for modern tailor made composite * Corresponding author: Friedrich Suchomel, Dr., research fields: cellulosic fibers, fiber reinforcement and green materials. E-mail: f.suchomel@lenzing.com. materials [4]. The major problems of natural fibers in this respect are the lacking purity as remaining organic substances like lignin or hemicellulose can influence the performance of the final composite part negatively like the resistance to elevated temperature. The mechanical properties are strongly dependent on the growth conditions and the climate thus leading to changing properties of natural fibers depending on the time of the harvest. Lenzing AG has developed TENCEL®—a sustainable fiber overcoming all these issues. The raw material for TENCEL® is wood, which is transformed into a fiber of pure cellulose. In a LCA (life cycle assessment) the environmental impact of Lenzing fibers was compared to cotton, PP (polypropylene) and PET (polyester). In this LCA 11 environmentally relevant factors have been evaluated and it has been shown that the environmental impact of Lenzing fibers is the lowest of all fibers in this study [5]. Due to the manufacturing process of TENCEL® the TENCEL®—A High-Performance Sustainable Cellulose Fiber for the Construction Industry/Composites 627 diameter is kept constant, thus mechanical properties like tensile strength or elongation vary only very little from one lot to the next. The various types of TENCEL® fibers are produced in a diameter range of 9-12 µm which is at least two times lower than the diameter of natural fibers giving at least four times the fiber amount per weight unit thus enhancing the reinforcement. The fiber dispersion depends not only on the fiber dimensions but can also be strongly influenced by the surface. Due to the production process the surface of TENCEL® can be modified and therefore adjusted to give optimum fiber dispersion. Due to all these properties the sustainable cellulosic fiber TENCEL® plays an important role in modern tailor made composite materials. 2. Experimental Section Due to the production process, the fiber is obtained as a tow which is then cut to length ranging from 34 mm to 60 mm based on the requirements for the further processing in the textile chain. Depending on the end-use of the fiber in the construction industry or composite materials the length had to be further reduced, either by cutting the fiber directly in the plant for lengths longer than 1 mm (TENCEL® short cut) or by using a cutting mill for the shorter length from 300 µm to 1 mm (TENCEL® FCP). The fibers used in the following experiments were 9, 10 or 12 µm in diameter, respectively. 2.1 Experimental Setup Concrete In the first experiments the optimum fiber length for the use in concrete was determined. As 6 mm and 12 mm TENCEL® fibers showed the best results in concrete all other experiments were made with such fibers. The experiments were all made first in a laboratory having precise control during the experiment and then the experiments were performed in concrete mixing plants or directly at construction sites to evaluate the practical implications of TENCEL® on the product quality and the workability of concrete. In the first series of experiments always two types of concrete, one with TENCEL® and one without were prepared and evaluated. In the more advanced experiments three concrete types, one without fibers (reference concrete), one with TENCEL® and one with polypropylene fibers were compared. The properties of concrete have to be divided in two distinct phases, the first being the fresh concrete phase and the second the hardened concrete phase, marking the final product of concrete. In the fresh concrete phase the focus lies on workability of the concrete, i.e., how well does the concrete flow or if any problems during the hardening stage can arise. Concrete in the cured state is the most abundant construction material in the world nowadays, there the focus lies mainly on properties like compressive or tensile strength. TENCEL® fibers are cellulosic fibers and therefore one of the main properties of TENCEL® fibers is the moisture management, i.e., the fast water uptake and slower release during the curing period of the concrete. This is the reason why the first experiments were designed to evaluate the influence of TENCEL® on the cohesiveness of concrete, the tendency to segregate and bleed, also under static pressure as exerted by the loads of the building on the foundation. This experiment is carried out by placing the fresh concrete in a container of known volume and applying a pressure of 3 bar for the period of an hour collecting the filter press water into a measuring cylinder (Fig. 1). The amount of water is recorded every 5 min and compared to other concrete types. This experiment was carried out with a TENCEL® content of 0.5, 1 and 1.5 kg/m³ concrete, equaling 0.02%, 0.04% and 0.06% per weight, respectively. With the concentration of 1 kg fibers per cubic meter of concrete, TENCEL® was compared with a stabilizer commonly used for such a purpose. Crack formation during curing of the concrete (early crack formation) is an issue for concrete constructions, mainly for large concrete slabs as the cracks in the 628 TENCEL®—A High-Performance Sustainable Cellulose Fiber for the Construction Industry/Composites (a) (b) Fig. 2 Shrinking of concrete: (a) crack formation; (b) test apparatus. Fig. 1 Filter press for testing concrete stability. concrete simplify corrosion attacks on the whole concrete slab and thus are to be prevented. Again, the moisture management of TENCEL® compared to PP fibers should have a positive impact on concrete curing. A simple, yet powerful method to evaluate the early crack formation of concrete are so-called shrinkage rings (Fig. 2) where the fresh concrete is filled in and stored for 8 h while subjected to a draught of 4 m/s (simulating a breeze) at 20 °C. After this curing time the length of the formed cracks is measured and an overall length is calculated as sum of the formed cracks. The average width is calculated by measuring the crack width at defined intervals and averaging the values. The crack area is defined as the product of the crack length and the average crack width. For this experiment three different concrete types were prepared, one without any fibers (reference concrete), one concrete with 1.2 kg/m³ PP fibers and one concrete with 1.2 kg/m³ TENCEL®. All three concrete types were filled into the rings and analysed according to the procedure described above. Concrete always contains some water; this water expands to water vapour when buildings like tunnels burn and thus leading to spalling of the concrete which in turn can cause the collapse of the whole building when the steel reinforcement melts. To prevent these events a common procedure in some European countries is the addition of PP fibers to concrete as these fibers melt during a fire leaving open pore space where the water vapour can expand [6]. As TENCEL® decomposes at a lower temperature than PP melts the performance of TENCEL® as a spalling prevention should be as good as PP fibers. Again, three kinds of concrete are tested, a reference concrete and two concrete types with 1.2 kg/m³ TENCEL® and PP, respectively. Then concrete slabs measuring 30 cm × 25 cm × 10 cm were cast containing thermo elements at defined intervals. The slabs were put in an oven in such a way that only one side was subjected to the fire while the other side was at room temperature. The temperature was increased until 1,153 °C in 4 h based on the EN 1363-1 unless a spalling event occurred before. 2.2 Experimental Setup Plastic Reinforcement Following boundary conditions had to be taken into account during the development process of TENCEL® FCP for reinforcing thermoplastic matrices: (1) Reinforcing the plastic material (L/D ratio); (2) Processability on compounding machines (dosing); (3) Smooth surfaces of the final injection moulded TENCEL®—A High-Performance Sustainable Cellulose Fiber for the Construction Industry/Composites 629 part (sufficient dispersion); (4) Uniformity of mechanical and dimensional properties of the fibers. First experiments where set up to evaluate the reinforcing potential of the fibers in polypropylene parts. Fibers taken for this trials have been TENCEL® FCP with a diameter of 10 µm and a length of 400 µm (L/D = 40), TENCEL® FCP with 35 µm and a length of 350 µm (L/D = 10) and for reference purposes a commercial available pulp length of 400 µm (average diameter 20 µm). In the next step the dosing behavior of the fibers was evaluated as the production process of thermoplastic compound materials requires quick adding of the fiber material. For this purpose a hopper equipped with an agitator was used. The hopper was filled with the different fibers and the flow behavior of the fiber was observed visually. The dispersion of the fibers in the plastic compounds was measured using a 3D computer tomography system (RayScan 250E) as this method allowed a non-destructive analysis of the plastic compounds showing the fiber distribution in the compound in detail. 3. Results and Discussion 3.1 Results Concrete The results from the filter press (cohesiveness) are summarized in Fig. 3 as obtained from concretes mixed in the lab as well as from large scale trials carried out in concrete mixing plants. As the filter press tests simulates the pressure of the surrounding areas on the concrete filled into holes for piling purposes, the less water is collected, the better the performance of the concrete in question. The loss of water in the concrete also leads to removal of the fine aggregates and thus can lead to a reduced stability of the concrete. The improved cohesiveness in comparison to reference concrete can be clearly seen as more water is collected from the reference concrete than from the concrete containing TENCEL®. The performance of TENCEL® is similar to a conventional stabilizer indicating that the sustainable TENCEL® fibers can be used as a replacement for a chemical stabilizer normally used in the concrete industry. In Fig. 4 the effect of TENCEL® on the early crack formation is clearly visible. Although the crack length 45 One of the most important topics when using fiber is the behavior under various environmental conditions like rain or UV radiation. For that reason the specimens where tested according to EN ISO 4892-2 where the reinforced plastic parts are 40 water amount [l/m³] reinforcement 35 Reference 30 25 stabiliser (2,4 kg/m³) 20 TENCEL (1 kg/m³) 15 10 5 exposed for 1,500 h to UV radiation and humidity 0 0 10 20 simulating changing weather conditions. Two matrix materials have been selected for this test. One was polypropylene, the other one was polylactic acid. For 30 40 120% reference concrete PP 100% TENCEL® FCP were prepared. In order to obtain also inspection mechanical tests like tensile strength, TENCEL® 6mm crack values PLA was also subjected to this test. In addition to visual 80% 60% 40% impact strength, flexural strength and impact strength 20% notched were performed as these tests are typically 0% performed for the determination of the performance of plastic parts. 60 Fig. 3 Filter press results—TENCEL® showing same performance as conventional stabilizer. both matrix materials compounds containing 30% the behavior of the pure matrix material, virgin PP and 50 time [min] crack length crack width crack area Fig. 4 Crack formation of concrete—comparison between PP and TENCEL®. 630 TENCEL®—A High-Performance Sustainable Cellulose Fiber for the Construction Industry/Composites is the same for TENCEL® and PP, the crack width using TENCEL® is considerably reduced compared to PP fibers. The early crack formation is a common problem in concrete technology, mainly when building large floors (e.g., for industrial purposes). As these lab results are promising large concrete floors have been made using TENCEL®. The first results showed a low crack formation and an improved surface quality. Further studies will carried out during the lifetime of the floor as often cracks form after some time (1-2 years). (a) In Fig. 5a the spalling effect of concrete exhibited to fire can be clearly seen, while in Fig. 5b the positive effect of TENCEL® is evident. The results from the fire experiments show that TENCEL® performs as well as PP fibers commonly used in concrete for spalling prevention. Further studies with other fire curves like the RWS (Rijkswaterstaat) curve are planned as this fire curve simulates the worst case of an oil containing truck which starts to burn inside a tunnel where the temperature rises to 1,140 °C in only 5 min and the maximum temperatures reach 1,340 °C. 3.2 Results Plastic Reinforcement (b) Fig. 5 (a) Spalling of conventional concrete after fire testing; (b) No spalling of concrete with TENCEL(R)® after fire test. In Fig. 6 the influence of the L/D-ratio on the tensile 15 µm lead to fibers longer than 500 µm resulting in 100 50 80 45 40 difficulties dosing such fibers. The main problem of 35 longer fibers could be observed as bridging behaviour in 30 the hopper. In addition longer fibers lead to a lower bulk 60 40 FCP 35/350 It can be clearly seen that fiber diameters higher than 55 pulp diameter of the fibers in question is depicted. 120 FCP 10/400 and the required fiber length taking the average Tensile strength in N/mm² the relationship between the desired L/D-ratio of 40 no. of fibers 60 no. of fibers in millions/g Tensile strength of compound (20%) strength of the plastic compound can be seen. In Fig. 7 20 - 5 10 15 20 25 30 35 40 45 50 55 60 Diameter in µm density and therefore to a lower dosing speed and thus a Fig. 6 Influence number of fibers on reinforcement. lower production capacity of the plastic compounds. As seen in Fig. 8. In Fig. 9 the impact of a lacking fiber distribution on the plastic part can be clearly seen. On been produced showing no surface effects while the part on the right side contains a standard natural fiber (coarser than TENCEL®) exhibiting a lower dispersion and forming agglomerates which tend to for production needs the fiber length should be as low as possible, only fibers having diameters lower than 15 µm are of interest showing a sufficient L/D-ratio and a reasonable production capacity. The excellent fiber dispersion of TENCEL® can be TENCEL®—A High-Performance Sustainable Cellulose Fiber for the Construction Industry/Composites 631 Target: L/D ≥ 1/30 for optimal reinforcement L/D = 40 2500 fiber length [µm] 2000 glass fiber, TENCEL FCP 1500 flax, hemp, Pulp 1000 500 0 0 10 20 30 40 50 60 fiber diameter [µm] Fig. 7 L/D-ratio and resulting fiber length for different fiber types. Fig. 8 3D CT pictures of a test bar; 20% TENCEL® FCP in PP. break through the outer layer of the polymer. In the magnification this effect is clearly visible. All these factors together make TENCEL® an excellent reinforcing fiber as can be seen in Fig. 10 where several mechanical properties are compared between pure PP and PP reinforced with TENCEL®. After the weathering tests the reference specimen made from pure PP showed nearly no change in the Young modulus, however the tensile strength was reduced by 50% of the initial value. Referring to the reinforced samples it can be stated that the modulus behaved in the same way. Concerning the tensile strength a reduction of approximately 13% was observed. As this reduction in tensile strength is also observed for pure PP parts after the weathering tests, it can be deduced that TENCEL® itself is not degraded during the weathering. On the opposite, using TENCEL® as a reinforcement of PP parts leads to an improved performance of such parts even after weathering. 4. Conclusions The results obtained with TENCEL® in such different areas of applications like reinforcing plastic composites and construction materials like concrete or plaster show that TENCEL® can play an important role in the ever increasing demand for optimized Fig. 9 Left: part made from TENCEL®, right: part made from conventional natural fiber. Tensile modulus requirements for reinforcing plastic compounds or pure PP improving the quality of construction materials but as a PP + 30% FCP sustainable and natural fiber has an excellent position 250% 200% HDT-A 150% 100% Tensile strength 50% for manufacturing sustainable goods. TENCEL® is under constant development for further improving modern composite materials like 0% exploring the potential of incorporating active Flexural modulus Impact strength notched materials. TENCEL® fulfills not only the technical Flexural strength Fig. 10 Comparison mechanical properties between pure PP (basis 100%) and PP reinforced with TENCEL®. ingredients or new surface modifications to enhance the properties of modern composite materials. Acknowledgments The authors thank Mr. Salaberger from FH Wels for making the CT images of the plastic parts. 632 TENCEL®—A High-Performance Sustainable Cellulose Fiber for the Construction Industry/Composites References [1] [2] [3] Balaguru, P. Contribution of Fibers to Crack Reduction of Cement Composites during the Initial and Final Settling Period. ACI Material Journal 1994, 91, 280-288. Eichhorn, S. J. Regenerated Cellulose Reinforced Plastics; Kluwer Academic Publishers: Norwell, Mass., 2004; pp 287-303. Xanthos, M. Functional Fillers for Plastics; Wiley-Vch, 2010. [4] [5] [6] Fuqua, M. A.; Huo, S.; Ulven, C. A. Natural Fiber Reinforced Composites. Polymer Reviews 2012, 52, 259-320. Shen, L.; Patel, M. K. 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