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The major use of nanocellulose particles as fillers or binders for films to date is that they provide a means of restraining the behavior of the nanoparticles. For example, nanocellulose when incorporated into films and even when formed into nanofibers can serve as effective binders that reduce or eliminate interparticle voids, thereby influencing film properties such as optical properties, mechanical properties, and barrier properties.
The effect of lipidic solvents on the barrier performance of flexible polymeric films is a major area of research and development interest (e.g., Arias et al. 2012, 2014; Santillan et al. 2013; Lin et al. 2014; Hashemipour and Neeser et al. 2015). However, there are relatively few reports in the literature that address the effects of polymeric additives on the permeability of elastic materials containing MFC as a reinforcing agent (Saw and Thirumkal et al. 2013). Saw and Thirumkal (2013) found that, with increasing OPP (octamethyl-p-terphenyl) and MFC content, the oxygen permeability of the film decreased. However, the addition of 8 wt % MFC with 2 wt % OPP does not provide a significant improvement in oxygen resistance over the thermoplastic coating MFCOEP5OPP-80. In a different study, they found that addition of 1 wt % MFC to thermoplastic filaments containing 1 wt % OPP decreased both oxygen permeability and moisture content. They used MFC to enhance optical clarity by eliminating extractives and other impurities in the surface of a polyamide filaments. In this study, the addition of MFC to the thermoplastic filament prevented the penetration of oxygen, which helps to prevent oxidization of the filament.
Nanocellulose films prepared with various surfactant agents, as discussed in the above section, are still in the early stages of scientific exploration and their use in packaging is yet to be developed. For instance, the cationic surfactant cetyl trimethyl ammonium bromide (CTAB) is widely used in the preparation of nanocellulose to control the surface charge and to ensure high purity of the cellulose product. It has been found that CTAB in low concentration can enhance the barrier properties of the nanocellulose films; however, in the case of higher CTAB concentration, the barrier performance was dramatically reduced (Table B). Two general strategies have been used to overcome the poor mechanical properties of nanocellulose films due to their lack of structural strength.
The following review provides an overview of the early efforts in fabricating nanocellulose-containing films and layers. The inclusion of nanofillers as additives in polymer-based matrices has been recognized as providing several advantages. The formation of a physically stable and tight network is less likely to occur in films prepared from mixtures of nanocellulose and a plasticized polymer, compared to those prepared from mixtures of nanocellulose and a thermoplastic polymer. This is because the free chain end of the polymer material can be caged and trapped in the internal network of the nanocellulose. Nanocellulose may also facilitate the formation of a gradient structure in the matrix when it is mixed with a non-compatibile polymer. For example, the formation of a stronger interface between the shell of nanocellulose and the matrix can be stimulated if the mixture has a larger fraction of a synthetic or natural polymer component than the nanocellulose. The formation of a gradient structure may be beneficial for forming a stable film and may improve a barrier function of the obtained film by increasing the difference in mobility of components within the matrix. Another advantage is that the compatibility with polymer-based matrixes is promoted when nanocellulose with a low degree of substitution is used. The use of a high-substituted nanocellulose can result in no interaction with the matrix and a structure of more loosely packed cellulose nanocrystals. The goal is to prepare a film with a low porosity, so that internal pores cannot be generated by the air or water vapor in the atmosphere. In addition, it is important to avoid generating any air bubbles within a nanocellulose-containing film or layer. In this way, the nanocellulose particles of a nanocellulose-containing film or layer can be protected from gas permeation, and physical damage and swelling can be inhibited. Thus, the film or layer becomes less likely to absorb moisture and is less likely to crack. Furthermore, less color and odor can be transferred to a wrapped material. The storage stability of a raw material can be improved by using a nanocellulose film or layer. Nanocellulose readily provides all of these advantages. It can be anticipated that more attention will be given to nanocellulose-containing films in the future for various commercial applications. The discussion will be supported by other work in this area that is still at early stages. Some of the work in this section may also represent key issues in the future, to which more attention will be given in subsequent papers in this special issue. A firm understanding of the mechanism of film formation, the thermodynamics and kinetics of these processes, and the material properties of the resultant films are still needed to ultimately achieve a process for commercial applications. The following sections will make a brief summary of these materials.
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