Mechanical enhancement of cellulose nanofibril (CNF) films through the addition of water-soluble polymers

In this work, water-soluble polymers were screened through solution casting and polyvinyl alcohol (PVA) and poly(2-ethyl-2-oxazoline) (PEOX) were found as reinforcement agents for cellulose nanofibril (CNF) films. Mechanical property increases of 99% in elastic modulus, 93% in the ultimate tensile strength (UTS) and 134% in the work of failure (WOF) were reported for TEMPO-oxidized cellulose nanofibrils (TOCNFs) with 0.44 mmol/g carboxylate groups and 15 wt% PVA. PEOX had a higher elastic modulus increase of 113%, yet lower UTS and WOF increases were found at 63% and 28%, respectively. Additionally, increases in UTS and elastic modulus were also seen in mechanically fibrillated CNFs and TOCNFs with higher carboxylate contents (1.5 mmol/g). The toughening mechanism was attributed to the formation of strong hydrogen bonding between the CNFs and the hydrophilic polymers added. The presence of such mechanisms was indirectly confirmed by tensile testing, zeta potential and rheology. Graphic abstract: [Figure not available: see fulltext.]