Self-standing cellulose nanofibril
(CNF) films are regarded
as
one of the promising alternatives to current petroleum-based packaging
materials mostly due to their ability to form dense self-assembled
structures exhibiting high gas barrier properties. Nonetheless, one
of the major obstacles to the commercialization of these materials
in packaging applications is the high cost of raw materials and production
energy. In this study, we created self-standing films of lignin-containing
cellulose nanofibrils (LCNFs) derived from a recycled old corrugated
cardboard (OCC) pulp that costs less than bleached softwood Kraft
(BSK) pulp and requires half as much energy for refining to obtain
the same quality of material. The low zeta potential (−3.83
mV) of OCC-derived LCNFs (OCC-LCNFs) resulted in aggregation of the
fibrils in aqueous suspension, leading to considerable unpredictability
in oxygen permeability (OP) values (coefficient of variation 36%).
The addition of 3 wt % (based on the dry weight of LCNFs) carboxymethyl
cellulose lowered the coefficient of variation to 16% with an average
OP of 1478 (cc.μm/m2.atm.day) at 80% relative humidity.
Because the OP was higher than that of the CNF film made from BSK-derived
CNF (BSK-CNFs), we demonstrated that ionic crosslinking with trivalent
aluminum ion or covalent crosslinking with polyamide epichlorohydrin
decreased the OP by 30% at 23 °C and 80% relative humidity while
also significantly enhancing the tensile strength and modulus. In
addition, the presence of lignin in OCC resulted in a relatively lower
water vapor permeability value in OCC-LCNF films compared to BSK-CNF
films. Moreover, OCC-LCNF films showed complete UV-shielding (200–400
nm) property. Overall, this work provides a new opportunity to exploit
a recycled and inexpensive source of CNFs to produce robust gas barrier
materials for packaging applications.