Substitution of nanoclay in high gas barrier films of cellulose nanofibrils with cellulose nanocrystals and thermal treatment

The aim of this study is to design a nanocellulose based barrier film. For this purpose, cellulose nanofibrils (CNFs) are used as a matrix to create an entangled nanoporous network that is filled with two different nanofillers: nanoclay (reference), i.e. the mineral montmorillonite (MMT) and the bio-based TEMPO-oxidized cellulose nanocrystal (CNC-T), to produce different types of nanocelluloses and their main physical and chemical features were assessed. As expected, films based on neat CNFs exhibit good mechanical performance and excellent barrier properties at low moisture content. The introduction of 32.5 wt% of either nanofiller results in a significant improvement of barrier properties at high moisture content. Finally, thermal treatment of a dried CNF/CNC-T film results in a decrease of the oxygen permeability even at high moisture content (>70 %). This is mainly attributed to the hornification of nanocellulose. A key result of this study is that the oxygen permeability of an all-nanocellulose film in 85 % relative humidity (RH), is similar to CNF film with mineral nanoclay (MMT), i.e. 2.1 instead of 1.7 cm³ µm m⁻² day⁻¹ kPa⁻¹, respectively.