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Conventional composite formulation of cellulose nanocrystals (CNCs) with thermoplastics involves melt compounding or in situ polymerisation. In this rather unconventional approach, polypropylene (PP) microparticles were finely suspended and stabilized, at varying weight loadings, in aqueous suspensions of amphiphilic CNCs to enable adsorption of the nanoparticles onto the thermoplastic. In order to achieve these suspensions, CNCs were modified with either octyl or hexadecyl groups. These modifications imparted hydrophobic properties to the CNCs, hence increasing interfacial adhesion to the PP microparticles. The modification, however, also retained the sulfate half ester groups that ensured dispersibility in aqueous media. The CNCs were evidently coated on the PP microparticles as revealed by confocal microscope imaging and had no detrimental effect on the melt properties of the PP-based composites. The approach is demonstrated to increase the Young’s moduli of CNC-thermoplastic composites prepared in optimum suspension loadings of 0.5 wt. % octyl-modified and 0.1 wt % hexadecyl-modified CNCs. This procedure can be extended to other thermoplastics as the ability to aqueously process these composites is a major step forward in the drive for more sustainable manufacturing.
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