Pulped Phormium tenax leaf fibres as reinforcement for epoxy composites

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Abstract

Leaf fibres from Phormium tenax (harakeke, New Zealand flax) were pulped at 170 °C with NaOH and anthraquinone. The pulp was wet laid to form mats, which were used to reinforce epoxy composites. The flexural modulus was almost as high as that measured for epoxy reinforced with glass chopped strand mat at the same weight fraction. The flexural strength was two-thirds that of the glass-reinforced composite. Failure was abrupt. SEM images showed torn fragments of fibre cell walls protruding from the fracture surface, indicating strong interfacial bonding. Good mechanical performance was attributed to the rarity of kink bands in the individual fibre cells, along with wrinkled cell-wall surfaces that enhanced the area of the fibre–matrix interface.

Introduction

Leaf fibres are often used to reinforce composite materials, primarily because of their low cost relative to bast fibres such as flax and hemp [1], [2]. Untreated leaf fibres provide little or no improvement in mechanical properties relative to unreinforced resin [3], [4], [5], [6], [7], [8]. Numerous chemical treatments have been studied [2]. Adding a binder, e.g., polyvinyl acetate, can enhance the reinforcing properties [9]. We assessed pulped leaf fibres as an alternative form of reinforcement.

Fig. 1 summarises flexural strengths reported for unsaturated polyester resins reinforced with untreated fibres from the leaves of three different species of plants [3], [4], [5], [6], [7], [8]. Unidirectional composites were excluded from this summary. Most of the data points for composites reinforced with abaca and/or sisal fibres showed no detectable strengthening. One study of sisal and two studies of pineapple leaf fibre (PALF) showed small improvements in flexural strength. Switching to an epoxy resin raised the flexural modulus for sisal-reinforced composites, without a significant improvement in strength [10].

The poor performance of leaf fibres might be associated with the fact that they are bundles of many fibre cells, often displaying 100 or more cells in a cross-sectional cut [1]. Only a small proportion of those cells contribute to the fibre–matrix interface. PALF bundle diameters, typically in the range 20–80 μm, are smaller than those for sisal bundle diameters, typically 50–200 μm [2]. The smaller diameters expose a higher proportion of fibre cells to the matrix, helping to account for the superior mechanical properties that are usually observed for PALF (Fig. 1). Further improvements in mechanical strength might be achieved by pulping leaf fibres to liberate the individual fibre cells, so that all of the cells contribute to the fibre–matrix interface. Duchemin et al. [11] tested that idea by pulping harakeke (Phormium tenax) leaf fibres at 170 °C, mixing the fibres with poly(lactic acid) and compression moulding. The composites were stronger than those reinforced with raw leaf fibres at the same fibre fractions. We extended that line of research by embedding harakeke leaf fibres in a thermosetting matrix.

Section snippets

Materials

Line fibre was obtained from the Templeton Flax Mill, Riverton, New Zealand. The fibre was stripped from the leaves of local wild plants. Pulping conditions were based on those published for leaf fibres from other species [12], [13], [14], [15]. Soda pulping is a redox process, in which the lignin is depolymerised by reduction while carbohydrates become oxidised [16]. Anthraquinone catalyses the process [16], and has been used in pulping leaf fibres [12], so we added it to the pulping liquor.

Fibre morphology

High-energy beating was avoided in production of the leaf-fibre mats, since the goal was to produce a network that would be readily penetrated by epoxy resin. Beating can produce felted networks that might be appropriate for paper products, but not reinforcing mats. The absence of felting was confirmed by FESEM images (Fig. 2), which showed individual fibre cells, linear or gently curved, packed in a loose random network. The structure of the network was similar to that in glass chopped strand

Conclusion

Pulping and wet-laying leaf fibres can enhance their potential for reinforcing thermoset resins, at least in the case of P. tenax fibres combined with epoxy resin. The flexural modulus can approach that of a composite reinforced by glass fibre, at a similar weight fraction, although the flexural strength falls short of that achieved with glass fibre. Compressive defects are less abundant in P. tenax fibres than in flax or hemp fibres, helping to account for the reinforcement properties of P.

Acknowledgements

The authors thank the Biopolymer Network Ltd. for funding under New Zealand Foundation for Research Science and Technology contract BPLY0402, Ananteshwar Vikram Singh for making and testing the glass fibre composite, Evan Sims for preparing the first batch of pulp, Jacqueline Bond and Anni Ratz for assistance with microscopy, Malcolm Daley for carbohydrate analyses, and James Carpenter and Eva Clauss for advice and assistance.

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