Strategies for Renewable Barriers with Enhanced Performance

Sammanfattning: Forest biomass is expected to play an increasingly important role in tomorrow´s global bio-economy as one of the main renewable sources of materials, chemicals and energy. In the framework of the biorefinery concept, the forestry industry is looking for new processes to utilize several fractions in the biomass (cellulose, hemicelluloses, lignin etc.), thereby generating value-added by-products, an economically sustainable process, and new market opportunities. The work presented in this thesis aims to develop oxygen barrier films and coatings based on the hemicelluloses-rich biorefinery fraction, referred to as wood hydrolysate (WH). These WHs were obtained from the aqueous process liquor after the hydrothermal treatment of hardwood. The WH-based films and coatings are intended to meet the increasing demand of bio-based and biodegradable barrier materials in multi-layered laminates for the food-packaging sector. This work has employed four strategies to provide control and enhancement of the mechanical and barrier properties of WH: I) a selective choice of up-grading pre-treatments of the WH aqueous liquor, II) the incorporation of layer silicates into the barrier formulation, III) chain-extension of the hemicellulose chains present in the WH via reductive amination, and IV) the development of wood hydrolysate polyelectrolyte complexes (PEC) with quaternized cellulose (QC). It has been demonstrated that the crude WH, with almost no upgrading pre-treatment, produced coatings with the best performance in terms of low oxygen permeability. Furthermore, the addition of naturally occurring layered silicates into the WH-based film formulations led to a decrease in water vapor permeability, and a considerably lower oxygen permeability at 80% relative humidity. Moreover, the chain-extension approach was shown to significantly enhance the formability and mechanical performance of WH-based films, making it possible to produce cohesive films with a higher proportion of WH, 70–85% (w/w) and to reduce the content of co-components in the films. The WH/QC-PEC-based films exhibited by far the best tensile properties, better than those previously obtained with carboxymethyl cellulose as a co-component in an equal amount, with a tensile strain-at-break as high as 7 %.