Janak Sapkota

Reinforcing Poly(ethylene) with Cellulose Nanocrystals

The fabrication of nanocomposites of low-density polyethylene (LDPE), one of the worlds most widely used polymers, and cellulose nanocrystals (CNCs), which represent the worlds most abundant bio-based nanofiller, is reported. While the hydrophobic polymer and the hydrophilic filler seem to be intrinsically incompatible, this article shows that it is possible to kinetically trap homogeneous nanocomposites by a templating approach. An organogel is first prepared by exchanging the solvent of an aqueous CNC dispersion against acetone, impregnating the resulting organogel, in which the CNCs form a percolating network with a hot LDPE solution in toluene, and compression-molding the resulting materials into thin films. At a filler content of 7.6% v/v, the resulting materials display a three- to four-fold increase in strength and stiffness compared with the neat LDPE, which confirms that the CNC network could be largely maintained. It is also possible to reprocess these nanocomposites and dilute them with LDPE using conventional melt-processing techniques.

Polymer Nanocomposites with Cellulose Nanocrystals Featuring Adaptive Surface Groups

Cellulose nanocrystals (CNCs) are mechanically rigid, toxicologically benign, fiber-like nanoparticles. They can easily be extracted from renewable biosources and have attracted significant interest as reinforcing fillers in polymers. We here report the modification of CNCs with the 2-ureido-4[1H]pyrimidinone (UPy) motif as an adaptive compatibilizer, which permits the dispersion of UPy-modified CNCs in nonpolar as well as polar media. In toluene, the UPy motifs appear to form intra-CNC dimers, so that the particles are somewhat hydrophobized and well-dispersible in this nonpolar solvent. By contrast, the UPy motifs dissociate in DMF and promote dispersibility through interactions with this polar solvent. We have exploited this adaptiveness and integrated UPy-modified CNCs into nonpolar and polar host polymers, which include different poly(ethylene)s, a polystyrene-block-polybutadiene-block-polystyrene elastomer and poly(ethylene oxide-co-epichlorohydrin). All nanocomposites display an increase of stiffness and strength in comparison to the neat polymer, and some compositions retain a high elongation at break, even at a filler content of 15% w/w.