Enhanced homogeneity and interfacial compatibility in melt-extruded cellulose nano-fibers reinforced polyethylene via surface adsorption of poly(ethylene glycol)-block-poly(ethylene) amphiphiles

In this paper, we demonstrate that an amphiphilic block copolymer such as polyethylene glycol-b-polyethylene can be used as both dispersing and interfacial compatibilizing agent for the melt compounding of LLDPE with cellulose nano-fibers. A simple and effective spray drying methodology was first used for the first time for the preparation of a powdered cellulose nano-fibers extrusion feedstock. Surface adsorption of the amphiphilic PEG-b-PE was carried out directly in solution during this process. These various dry cellulosic feedstock were subsequently combined with LLDPE via extrusion to produce a range of nano-composites. The collective outcomes of this research are several folds. Firstly we show that presence of surface adsorbed PEG-b-PE effectively hindered the aggregation of the cellulose nano-fibers during the extrusion, affording clear homogenous materials with minimum aggregation even at the highest loading of cellulose nano-fibers (∼23 vol.%). Secondly, the tailored LLDPE/cellulose interface arising from intra- and inter-molecular hydrogen and Van der Waals bonds yielded significant levels of mechanical improvements in terms of storage and tensile modulus. We believe this study provides a simple technological template to produce high quality and performant polyolefins cellulose-based nano-composites.