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Terzi, E., Kartal, S., Muin, M., Hassanin, A., Hamouda, T., Kılıç, A., and Candan, Z. (2018). "Biological performance of novel hybrid green composites produced from glass fibers and jute fabric skin by the VARTM process," BioRes. 13(1), 662-677.

Abstract

Environmentally friendly composites are increasingly used in building applications that require fungal and insect resistance. This study evaluated the ability of both wood-degrading and mold fungi to decompose hybrid composites made of wood furnish, glass fibers, and jute fabric skin. Fungal decay resistance tests employed brown-rot fungus (Fomitopsis palustris) and white-rot fungus (Trametes versicolor). Mold resistance tests were performed with a mixture of three mold fungi, Aspergillus niger, Penicillium chrysogenum, and Trichoderma viride. The test specimens were also bio-assayed against termites in both laboratory and field conditions. When compared to control composites specimens produced by conventional methods without glass fiber and jute, the specimens with/without glass fiber and jute fabric manufactured by the VARTM process showed high resistance against the wood-degrading fungi and termites under laboratory and field conditions; however, mold fungal growth was observed on the surfaces of the specimens with 10%, 15%, and 20% glass fiber (without jute fabric) and with 5%, 10%, and 15% glass fiber (with jute fabric). In geographical locations with severe decay and termite hazards, these composite products may have a long service life as alternatives to conventional composites.


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Biological Performance of Novel Hybrid Green Composites Produced from Glass Fibers and Jute Fabric Skin by the VARTM Process

Evren Terzi,a,*S. Nami Kartal,a Musrizal Muin,b Ahmed H. Hassanin,c,e Tamer Hamouda,d Ali Kılıç,e and Zeki Candan a

Environmentally friendly composites are increasingly used in building applications that require fungal and insect resistance. This study evaluated the ability of both wood-degrading and mold fungi to decompose hybrid composites made of wood furnish, glass fibers, and jute fabric skin. Fungal decay resistance tests employed brown-rot fungus (Fomitopsis palustris) and white-rot fungus (Trametes versicolor). Mold resistance tests were performed with a mixture of three mold fungi, Aspergillus nigerPenicillium chrysogenum, and Trichoderma viride. The test specimens were also bio-assayed against termites in both laboratory and field conditions. When compared to control composites specimens produced by conventional methods without glass fiber and jute, the specimens with/without glass fiber and jute fabric manufactured by the VARTM process showed high resistance against the wood-degrading fungi and termites under laboratory and field conditions; however, mold fungal growth was observed on the surfaces of the specimens with 10%, 15%, and 20% glass fiber (without jute fabric) and with 5%, 10%, and 15% glass fiber (with jute fabric). In geographical locations with severe decay and termite hazards, these composite products may have a long service life as alternatives to conventional composites.

Keywords: Green composites; Hybrid composites; Biological performance; Decay; Termite; Mold

Contact information: a: Department of Forest Industrial Engineering, Faculty of Forestry, Istanbul University, Istanbul, Turkey; b: Hasuniddin University, Indonesia; c: Department of Textile Engineering, Alexandria University, Alexandria, Egypt; d: Textile Research Division, National Research CentreDokki, Giza, Egypt; e: TEMAG Labs, Faculty of Textile Technology and Design, Istanbul Technical University, Istanbul, Turkey; *Corresponding author: evrent@istanbul.edu.tr

INTRODUCTION

Biodegradable and renewable composites are a response to the important issues of sustainability and environmental impact. The use of renewable resources, such as plant-based materials, reduces the dependence on shrinking natural resources such as wood (Satyanarayana 2015). Plant-derived composites, i.e., lignocellulosics, have numerous applications and are being converted into value-added materials (Ashori 2008; Shah 2013; Hamouda et al. 2015, Garcia-Garcia et al. 2016; García et al. 2016; Hassanin et al. 2016a; Katogi et al. 2016; Nurul Fazita et al. 2016; Wang and Shih 2016).

Due to their biological nature, lignocellulosic composite materials are susceptible to attack by microorganisms (Curling and Murphy 1999; Kartal and Green III 2003). Although environmentally friendly composites are likely to have acceptable mechanical and physical properties compared with other conventional wood-based composites, their biological performance is important when they are used in harsh environments. The biological resistance of composites highly depends on fibers, fillers, resin, and other binding materials used in board manufacturing. The incorporation of naturally durable plant fibers in manufacturing processes may increase the resistance to biological attack (Barnes and Amburgey 1993; Evans et al. 1997; Kard and Mallette 1997; Evans et al. 2000; Kartal and Green III 2003). However, bio-composites also depend on resins and other binding materials for their integrity, and failure in these binding materials can greatly affect the resistance of the entire composite to biological degradation (Wagner et al. 1996; Vick et al. 1996; Carll and Highley 1999; Kartal and Clausen 2001). Renewable fiber-reinforced polymer composite materials are increasingly popular in various applications in construction, the automotive industry, etc. In addition to interior usage, the use of hybrid composites in particularly high-decay-hazard environments is likely to grow. However, little information is available on the resistance of fiber-reinforced hybrid composites to microbial biodegradation. Impurities, additives, fibers, and other materials in the production process may promote fungal and bacterial growth because such materials are a source of carbon and energy for microorganisms (Tascioglu et al. 2003).

This study evaluates the biological resistance of hybrid green composite boards previously tested for their mechanical and physical properties (Hassanin et al. 2016b). The core portion of the composite board was reinforced with short glass fibers. The prepared composites were also supported with woven jute fabrics. The vacuum assisted resin transfer molding (VARTM) technique was used to combine the core board and woven jute skin. Due to their high availability, glass fibers are generally used as reinforcement in fiber-reinforced composites. Jute is a cellulosic natural fiber and can be processed to manufacture diverse textiles, usually in the form of woven fabrics. In addition to their renewability, these natural plant fibers are non-toxic and cost-effective materials for composite products. In this study, fungal decay and mold resistance tests were performed in laboratory conditions. Both laboratory and field termite resistance tests were used to evaluate the insect resistance of the produced hybrid-composite boards.

EXPERIMENTAL

Materials

The particle mixture used to manufacture hybrid composites was composed of maritime pine (Pinus pinaster), mixed pine, oak (Quercus spp.), and poplar (Populus spp.) woods (25%, by weight) and was supplied by Kastamonu Integrated Wood Industry Inc., Gebze, Kocaeli, Turkey. Urea formaldehyde resin and ammonium chloride were used as a hardener.

Short glass fibers (12 mm) were also used as reinforcement. Unsaturated polyester resin (BRE310) was purchased from Boytek (Istanbul, Turkey). The final resin composition contained 0.5% w/w cobalt octate as the accelerator and 1 wt.% methyl ethyl ketone peroxide (MEKP) as the initiator. The jute fabric had a balanced plain weave 1/1 structure with an areal density of 280 g/m2.

Manufacturing Methods

Hybrid composites

Two main procedures were followed to produce hybrid composites. In the first, particleboards with an average target density of 310 kg/mwere prepared using the formaldehyde and wood particle-glass mixture, which was hot-pressed in mild conditions. The wood particle mixture was composed of maritime pine (Pinus pinaster, 45% by weight), mixed pine (35% by weight), oak, and poplar woods (20% by weight). The particles were mixed with urea formaldehyde resin and ammonium chloride as a hardener. The mixing procedure was repeated several times to ensure the distribution of the resin within the wood particles. Short glass fibers (12 mm) were used as reinforcement. In total, 10 filler compositions were prepared by mixing wood particles and short glass fibers at different ratios between 0% and 20% by weight. Mixing was repeated several times to ensure a homogenous distribution of the short glass fibers. Homogenously mixed mats were hot pressed at 8 bar and 180 °C for 7 min in a laboratory scale hot press. The obtained panels had dimensions of 40 mm x 40 mm x 10 mm. Particleboard panels were conditioned in a climate chamber at 65% relative humidity (RH) and 20 °C.

Table 1. Composition of Hybrid Green Composites

This process was followed by a second procedure, where the sandwich hybrid composites were prepared using the vacuum-assisted resin transfer molding (VARTM) technique in a closed mold. A detailed procedure is described in Hassanin et al. (2016a, b). Vacuum was applied to facilitate unsaturated polyester resin flow into the particleboard mat. After the impregnation, the composite cured at room temperature (Xia et al. 2015). Unsaturated polyester resin (BRE310) was purchased from Boytek (Istanbul, Turkey). The final resin contained 0.5% (w/w) cobalt octate as the accelerator and 1 wt.% methyl ethyl ketone peroxide (MEKP) as the initiator.

For the fabrication of hybrid composites, woven jute fabrics acquired from local stores were used as the skin layers. The jute fabric had a balanced plain weave 1/1 structure with an areal density of 280 g/m2. The obtained jute fabric had almost equal mechanical properties in both warp and weft directions. The average breaking force and extension for jute fabric in warp and weft directions were 526.5 N and 5.8%, respectively. Of the 10 composite groups, five were covered with jute fabrics. The samples were cured at room temperature for 25 min.

The compositions of the samples are given in Table 1. The samples were named according to presence of wood (W), short glass fibers (G), and jute (J). The first 5 samples did not contain a skin layer of jute fabric, whereas the top and the bottom layers of the next 5 were covered with woven jute fabrics by the VARTM process.

Conventional composites – controls

Conventional particleboard specimens to be served as controls were prepared using the traditional hot press technique. Particleboard panels were designed in a single layer with a target density of 660 kg/m3. The raw materials consisted of 65% softwood and 35% hardwood particles by weight. Urea-formaldehyde (UF) resin at the 10% adhesive level by oven-dry weight was used based on the oven-dry weight of wood particles. One-percent ammonium chloride (NH4Cl) by weight was added to the resin as a hardener. The particles were placed in a drum blender and sprayed with UF resin and NH4Cl for 5 min to obtain a homogenized mixture. The conventional composites had a thickness of 10 mm and an average density of 0.66 g/cm3.

Tests

Fungal decay resistance tests

Two Basidiomycetes—brown-rot fungus, Fomitopsis palustris (Berk. & M.A. Curtis) Gilb. & Ryvarden (TYP 0507), white-rot fungus, Trametes (Coriolus) versicolor (L.:Fr.) Pilat (COV 1030)—were used in decay tests. The decay resistance of composite specimens (20 mm × 20 mm × 10 mm) was evaluated by inserting the specimens directly into Petri dishes inoculated with Basidiomycetes fungi. Before decay testing, all specimens were dried at 60 °C for 3 days. The fungi were inoculated on 2% malt extract agar (MEA) in Petri dishes separately for 3 weeks at 23 °C before placement of the specimens into the dishes. The specimens were autoclaved at 121 °C and 15 psi for 20 min for sterilization and then placed into the inoculated Petri dishes. One specimen was placed in each dish, and conventional composite specimens served as controls. Sixteen specimens were used for each specimen group and each fungus. After a 12-week incubation period in a temperature and humidity-controlled chamber at 26 °C and 65% RH, the specimens were dried at 60 °C for 3 days and weighed to calculate weight losses based on the weights of the specimens before and after decay resistance tests.

Mold fungi resistance tests

Three mold fungi—Aspergillus niger 2.242, Penicillium chrysogenum PH02, and Trichoderma viride ATCC 20476—were used in mold tests. Composites by the VARTM process and control (conventional composites) specimens (20 mm × 70 mm x thickness) were evaluated for resistance to mold fungi according to a modified ASTM D 4445-10 (2015) protocol. The mold fungi were grown on 2% malt agar (Difco, Detroit, MI, USA) at 27 °C and 80% RH. All fungi were obtained from the USDA Forest Service Forest Products Laboratory, Madison, WI, USA. A mixed spore suspension of the three test fungi were prepared by washing the surface of individual 2-week-old Petri plate cultures with 10 to 15 mL of sterile DI water. Washings were combined in a spray bottle and diluted to approximately 100 mL with DI water to yield approximately 3 x 107spores/mL. The spray bottle was adjusted to deliver 1 mL of inoculum per spray. The specimens were sprayed with 1 mL of mixed mold spore suspension and incubated at 27 °C and 80% RH for 4 weeks. Following incubation, the specimens were visually rated on a scale of 0 to 5 with 0 indicating the specimen is completely free of mold growth and 5 indicating the specimen was completely covered with mold growth (0: no growth, 1: 20%, 2: 40%, 3: 60%, 4: 80%, 5: 100% coverage with mold fungi).

Laboratory termite resistance tests

The subterranean termites Coptotermes curvignathus Holmgren (Order Isoptera, Family Termitidae) were used in laboratory tests for termite resistance. The tests were carried out based on the Indonesian National Standard SNI 01.7207 (2006). Table 2 summarizes the test method in the mentioned standard.

Table 2. General Description of Laboratory Termite Resistance Tests

A composite specimen (25 mm × 25 mm × 10 mm) was placed in a glass jar, leaning against a sidewall with 200 g sand (7% moisture content under water holding capacity of the sand) and 200 healthy and active workers of C. curvignathus. Conventional composites and solid wood from Scots pine sapwood specimens served as controls. The jam pots were placed in a dark room for 4 weeks, and the bottles were weighted weekly to regulate the moisture content of the sand. In cases where the moisture content of the sand was reduced by 2% or more, water was added to reach the moisture content stated in the standard. Resistance to subterranean termites according to the Indonesian National Standard SNI 01.7207 (2006) is given in Table 3. Each test specimen was examined and visually rated using a rating system given in Table 4.

Table 3. Termite Resistance Classes Based on Weight Losses

Table 4. Rating System for Visual Evaluations of Termite Resistance*

Field termite tests

The tests were performed in South Sulawesi, Indonesia, which has an average annual rainfall of 2875 mm and annual temperature of 31 °C. The test area has a typical tropical climate and shows heavy attacks of Coptotermes sp. The exposure test involved laying a test specimen (20 mm × 10 mm × 100 mm) on top of hollow concrete blocks standing on the soil surface and then covering the structures with a PVC pipe cap to protect the sample from rain and to maintain high humidity. There was no direct contact between the specimen and the soil, other than that brought about by the termites to construct shelter tubes. Through the two perforations in each block, 25 mm × 25 mm × 300 mm pine (Pinus merkusii) feeder stakes were driven into the ground so that the top of the stake was within 2 to 5 mm of the top of the concrete block. The test specimens were situated one per block such that they covered the holes in the block but were not in direct contact with the feeder stake. This design prevented direct tunneling by termites from the untreated wood stakes into the test samples. Conventional composite specimens served as controls. After six weeks of exposure, each specimen was carefully removed, examined, and visually rated.

Statistical evaluations

Weight losses from decay and termite resistance tests and mold ratings were statistically analyzed by the Student’s t-test (inerSTAT-a v1.3) for the composite groups. One-way analysis of variance (ANOVA) was conducted by the inerSTAT-a V.1.3 program, and p and F values were calculated (Vargas 1999).

RESULTS AND DISCUSSION

The final thickness of the produced hybrid green composites was 10 mm, and their average density was 1000 kg/m3. This result confirmed that a sandwich structure with or without jute fabric layers bonded to the light particleboard core (density, 310 kg/m3) was constructed by the VARTM process.

The average weight losses of test specimens exposed to T. versicolor and F. palustris fungi for 12 weeks and the statistical significance among the composite groups are given in Fig. 1 and Table 5.

When compared to conventional composite specimens (controls), the hybrid composite specimens by the VARTM process showed apparently increased fungal resistance and those specimens had statistically significant differences (p<0.01). However, there was no close relationship between weight losses and types of the hybrid composites by the VARTM process.

Fig. 1. Weight losses after 12-week-fungal resistance tests (W: wood, G: short glass fibers, J: jute)

Weight losses in the hybrid composite specimens varied between 1.98% and 4.44%. In general, there were slightly higher weight losses in the specimens containing either glass fiber only or glass fiber plus jute fabrics than in the WR0G specimens. Statistically significant differences were observed in the specimens from the WR5G, WRG0J, WRG5J, and WRG10J composite groups compared with the WR0G specimens for all test fungi. However, increased glass fiber content in the specimens with jute fabric (WR20GJ) decreased the weight losses to the amounts similar to the WR0GJ specimens. In most specimens, jute fabric caused slight increases in weight losses compared with the non-fabric composite groups. According to ASTM D 2017-05 (2010) (Table 6), the hybrid green composite specimens by the VARTM manufacturing process were classified as “highly resistant” to the fungi tested even though this classification is generally applied to solid wood specimens.

Table 7 shows mold ratings in the specimens after a 4-week exposure to the mold fungi. The levels of statistical significance among the composite groups are given in Table 8.

Table 5. Statistical Evaluations of Weight Losses Occurred in the Composite Groups by the T. versicolor and T. palustris Fungi

According to the ASTM D 2017-05 (2010) Standard Test Method

Table 6. Decay Resistance Expressed Either Weight Loss or Residual Weight (ASTM 2010)

Table 7. Mold Ratings Occurred in the Composite Groups

Note: Mold growth rating in pine sapwood specimens: 5. Values in parentheses are standard deviations (n = 5).

The lowest mold growth rates were exhibited by specimens with the two lowest glass fiber contents without jute skin. Incorporation of glass fibers at 10%, 15%, and 20% loading levels increased mold growth in the specimens. In the specimens with jute fabric skin, the lowest mold growth rates were observed in both the lowest and highest glass fiber-containing specimens. The specimens with 5%, 10%, and 15% glass fiber and jute fabric and conventional composites as controls were completely covered by fungal growth at the end of the exposure period.

Average weight losses, visual evaluation ratings, and percentage survival of termites of the specimens during the termite bioassays (laboratory and field tests) and the levels of statistical significance among the composite groups (weight losses only) are shown in Tables 9 and 10, respectively.

Conventional composite specimens as controls showed much higher weight losses and lower V-rating and mortality values compared to the VARTM process-produced hybrid composites in both laboratory and field termite resistance tests. Thus, there were statistically significant differences (p<0.01) between conventional composites (controls) and hybrid composites by the VARTM process.

Table 8. Statistical Evaluations of Mold Ratings in the Composite Groups

There was no significant effect of specimen composition of the VARTM-produced specimens on the susceptibility of specimens to termite attack during the termite bioassays when compared with the WR0G specimens in both laboratory and field tests. Weight losses, termite survival, and visual ratings were at good accordance in both laboratory and field tests. According to the Indonesian National Standard SNI 01.7207 (2006), all specimens produced by the VARTM process were classified as “very resistant” to termites based on the weight losses (Table 3).

There were no direct comparisons available in the literature, as studies on hybrid composites generally employ different types of fibers, reinforcing materials, and additives, and they follow diverse production methods. Tascioglu et al. (2003) evaluated fungal degradation of glass fiber/phenolic resin containing composites. Their results demonstrated that there was no weight loss in test specimens exposed to white and brown rot fungi; however, the specimens were susceptible to fungal penetration.

Table 9. Laboratory and Field Termite Resistance Tests

Table 10. Statistical Evaluations of Weight Losses Occurred in Both Laboratory and Field Termite Resistance Tests

Gon et al. (2012) stated that the intensity of blackish spots on the surface of jute-reinforced composites increased with increasing humidity. A slight appearance of localized black spots on the surfaces of test specimens was seen at 85% RH and grew significantly at 95% RH and immersed water conditions. In various studies by Gu et al. (1995a, b; 1996; 1997; 2011), various additives in fiber-reinforced composites stimulated microbial growth. These components in the composite matrix serve as carbon, nitrogen, and energy sources for microorganisms (Tascioglu et al. 2003). Tascioglu (2003) showed that a melamine resin binder with a high nitrogen content may have promoted microbial degradation in test specimens produced from glass fiber. In the recent study, in most cases jute fabric in the specimens increased slightly weight losses in the decay resistance tests when compared to jute-free specimens. Similar results were obtained when the specimens were exposed to fungi, suggesting that jute fabric may slightly improve microbial growth on the specimen surfaces. The main chemical constituents of jute are alpha-cellulose, hemicelluloses, and lignin (Rowell and Stout 1998; 2006). Jute also contains minor constituents such as nitrogenous matter (0.8% to 1.5%) that might contribute to microbial growth.

CONCLUSIONS

  1. The hybrid composite specimens prepared by the VARTM process showed resistance against all decay fungi and termites in both laboratory and field tests when compared to control (conventional composites) specimens.
  2. Mold fungi were able to grow on some hybrid composite specimens with 10%, 15%, and 20% glass fiber without jute fabric and 5%, 10%, and 15% glass fiber with jute fabric and control specimens as well.
  3. Hybrid composite products may be useful in regions of severe decay and termite hazard, while mold fungi can grow on the surfaces of some specimen groups.

ACKNOWLEDGMENTS

The test specimens were kindly obtained from a previous study funded by the Scientific and Technological Research Council of Turkey (TUBITAK) under grant number 21514107-216.01-237755. This study was financially supported by The Coordination Unit for Scientific Research of Istanbul University, Turkey (Project No: BEK-2017-24435). This study was partly presented at the IRG 2017, Belgium.

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Article submitted: September 5, 2017; Peer review completed: October 29, 2017; Revised version received and accepted: November 19, 2017; Published: November 29, 2017.

DOI: 10.15376/biores.13.1.662-677