Nowadays, environmental pollution due to synthetic polymers represents one of the biggest worldwide challenges. As demonstrated in numerous scientific articles, plant-based nanocellulose (NC) is a biodegradable and nontoxic material whose mechanical, rheological, and gas barrier properties are competitive compared to those of oil-based plastics. However, the sensitivity of NC in humid ambient and lack of thermosealability have proven to be a major obstacle that hinders its breakthrough in various sectors including food packaging. In recent years, attempts have been made in order to provide a hydrophobic character to NC through chemical modifications. In addition, extensive works on nanocellulose applications in food packaging such as coating, layer-by-layer, casting, and electrospinning have been reported. Despite these enormous advances, it can easily be observed that packaging manufacturers have not yet shown a particular interest in terms of applicability and processability of the nanocellulose due to the lack of guidelines and guarantee on the success of their implementation. This review is useful for researchers and packaging manufacturers because it puts emphasis on recent works that have dealt with the nanocellulose applications and focuses on the best strategies to be adopted for swift and sustainable industrial manufacturing scale-up of high-performance bio-based/compostable packaging in replacement of the oil-based counterparts used today.

Cellulose nanocrystals (CNCs) exhibit outstanding gas barrier properties, which supports their use as a biobased and biodegradable barrier coating on flexible food packaging materials. As highly hydrophilic biopolymers, however, CNCs have a strong sensitivity to water that can be detrimental to applications with fresh foods and in moist conditions due to the loss of barrier properties. In this work, the oxygen and water vapor permeability of polyethylene terephthalate (PET) films coated with CNCs obtained from cotton linters were measured at varying levels of relative humidity, both in adsorption and desorption, and from these data, the diffusion and solubility coefficients were estimated. Therefore, the characterization of CNCs was aimed at understanding the fundamentals of the water-CNCs interaction and proposing counteractions. The CNCs' moisture absorption and desorption isotherms at 25 • C were collected in the range of relative humidity 0-97% using different techniques and analyzed through GAB (Guggenheim-Anderson-de Boer) and Oswin models. The effects of moisture on the water status, following the freezable water index, and on the crystal structure of CNCs were investigated by Differential Scanning Calorimetry and by X-ray Powder Diffraction, respectively. These findings point to the opportunity of coupling CNCs with hydrophobic layers in order to boost their capabilities as barrier packaging materials.

In this work, three types of cellulose nanocrystals (CNCs) were used: CNCSO3H extracted from wood pulp by sulfuric acid (H2SO4), CNCCOOH extracted from cotton linters by ammonium persulfate (APS) and CNCCOOR obtained by esterification of the previous two CNCCOOH and CNCSO3H. For a comparative assessment of gas barrier performance, plastic films such as PLA, PET, PE, PP, OPP and OPA were selected, coated with the three types of CNCs and finally laminated with a solvent-based polyurethanic adhesive. First, all dispersed CNCs were characterized by apparent hydrodynamic diameter and Z potential by means of dynamic light scattering (DLS) and electrophoretic light scattering (ELS) techniques, respectively, followed by the crystallinity index (XRD), thermogravimetric analysis (TGA) and evaluation of Fourier-transform infrared spectroscopy (FTIR), as well as the charges density. The surface chemistry of coated plastics (CNCs-P) was assessed by the Z potential through the electrokinetic technique (streaming potential method) and the optical contact angle (OCA). Lastly, laminated films (P-CNC-P) were evaluated by gas permeability measurements at 23 °C and 50–80% RH. It is worth noting that improvements between 90% and 100% of oxygen barrier were achieved after the lamination. This paper provides insights on the choice of cellulosic nanomaterials for the design and development of advanced and sustainable food packaging materials.

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