Controlling interfacial interactions in LDPE/flax fibre biocomposites by a combined chemical and radiation-induced grafting approach

By combining chemical and gamma radiation treatments, we show that it is possible to improve the interfacial adhesion between natural fibres and a non-polar and non-reactive matrix such as low density polyethylene (LDPE), and the resulting mechanical performances of their biocomposites. To this aim, flax fibres are first functionalized with octadecylphosphonic acid (ODPA) and the quantity, effective grafting and localization of ODPA molecules on flax fibres are characterized by ICP-AES, solid state ³¹P NMR and SEM-EDX. ODPA molecules are effectively grafted onto flax fibres at a content of roughly 2.5 wt% and mostly localized at the fibre surface. Moreover, contact angle measurements as well as water sorption kinetics give evidence for increased hydrophobic and oleophilic character of ODPA treated fibres. Pellets of LDPE/flax fibre biocomposites obtained by melt extrusion are then submitted to gamma radiation and processed by injection moulding. Based on Soxhlet extraction experiments and SEM observations, it is shown that LDPE cross-linking rate induced by gamma radiation is locally enhanced at the fibre/matrix interface, suggesting that regio-selective cross-linking occurred between LDPE chains and the alkyl chain of ODPA grafted on flax fibre surface. Consequently, the uniaxial tensile performances of the biocomposites are enhanced by this combined chemical and radiation-induced grafting approach, especially their ultimate properties (up to 40% increase in the work of rupture). These results evidence an enhanced interfacial adhesion that is also supported by more cohesive interfacial failure and higher work of rupture through in-situ micro-mechanical tensile SEM experiments.