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  • 1.
    Ibn Yaich, Anas
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology.
    Strategies for Renewable Barriers with Enhanced Performance2015Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    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 %.

  • 2.
    Ibn Yaich, Anas
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology.
    Wood hydrolysate Barriers2012Licentiate thesis, comprehensive summary (Other academic)
    Abstract [en]

    Wood hemicellulose is an abundant but fairly unexploited renewable feedstock. Recent studies have shown that hemicelluloses have a large potential for use in the food packaging industry as a sustainable alternative to the conventional oxygen-barrier materials used today. Such hemicelluloses are the main components of wood hydrolysates (WH), which are released in large quantities in many forestry process side streams. Recovering these hemicellulose-rich WH fractions and turning them into food packaging materials would be beneficial from both, an environmental and an economic point of view. However, in the development of packaging materials for large-scale applications, the high production costs to obtain the highly purified hemicellulose and their high moisture sensitivity are considered to be the two main limiting factors.In this study, a selective choice of the upgrading conditions during the recovery of WH and the incorporation of layered silicate particles in WH-based films and coating formulations are used as tools to control and tailor the barrier and tensile performances of the materials, enabling the design of renewable oxygen-barrier materials that are cost-effective and with improved properties. The WH originated from the aqueous liquor from hardwood hydrothermal treatment and upgraded according to one of three alternative routes (ultrafiltration, ultrafiltration followed by diafiltration, and ethanol precipitation) resulting in hemicellulose-rich fractions with different structures, compositions, and properties, which in turn resulted in different performances in terms of mechanical and oxygen-permeability properties. WH in its crudest form gave rise to coatings with the best oxygen-barrier performance, higher than the oxygen-barrier performance of pure hemicellulose coatings. The addition of montmorillonite or talc layered silicates as mineral additives in the WH-based films resulted in better water-vapor-barrier properties, and considerably improved oxygen barrier performance at a relative humidity as high as 80 %. The application of the WH-based films was therefore extended to a wider range of relative humidity conditions.

  • 3.
    Ibn Yaich, Anas
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology.
    Edlund, Ulrica
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology.
    Albertsson, Ann-Christine
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology.
    Adapting wood hydrolysate barriers to high humidity conditions2014In: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 100, p. 135-142Article in journal (Refereed)
    Abstract [en]

    The incorporation of layered silicates in bio-based barrier films resulted in lower water vapor permeability, and significantly lowered oxygen permeability at a relative humidity (RH) as high as 80%, with reduced moisture sensitivity of the wood hydrolysate (WH) based films. The applicability of WH based films was accordingly extended over a wider relative humidity condition range. Crude aqueous process liquor, the WH, was extracted from hardwood and utilized as a feed-stock for films without any upgrading pretreatment, yet producing superior oxygen barrier performance compared to partially upgraded WH and highly purified hemicelluloses. Films composed of crude WH and either one of two types of naturally occurring layered silicates, montmorillonite (MMT) or talc, as mineral additives, were evaluated with respect to oxygen and water vapor permeability, morphological, tensile and dynamic thermo-mechanical properties. Films with an oxygen permeability as low as 1.5 (cm(3) mu m)/(m(2) day kPa) at 80% RH was achieved.

  • 4.
    Ibn Yaich, Anas
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology.
    Edlund, Ulrica
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology.
    Albertsson, Ann-Christine
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology.
    Barriers from wood hydrolysate/quaternized cellulose polyelectrolyte complexes2015In: Cellulose (London), ISSN 0969-0239, E-ISSN 1572-882X, Vol. 22, no 3, p. 1977-1991Article in journal (Refereed)
    Abstract [en]

    Biobased polyelectrolyte complexes (PECs) were prepared by mixing negatively charged O-acetyl-4-O-methylglucuronoxylan-rich wood hydrolysate (WH) and positively charged quaternized cellulose (QC) in aqueous solution. The WH was obtained as an aqueous process liquor of the hydrothermal treatment of birch wood chips and partially upgraded by membrane filtration and dialysis. Three QC derivatives with different degrees of quaternization were synthesized, characterized in terms of molecular weight, charge density, crystallinity and solubility, and utilized for PEC production. The WH/QC PECs were designed to form free-standing films with high oxygen barrier performance and good mechanical integrity. The impact of the QC degree of quaternization on the oxygen permeability at both 50 and 80 % relative humidity, water vapor permeability and tensile properties was investigated. Films with a tensile strain-to-break as high as 7 % and an oxygen permeability as low as 1.3 (cm(3) mu m)/(m(2) - day kPa) at 80 % relative humidity were achieved.

  • 5.
    Ibn Yaich, Anas
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
    Edlund, Ulrica
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
    Albertsson, Ann-Christine
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
    Enhanced formability and mechanical performance of wood hydrolysate films through reductive amination chain extension2015In: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 117, p. 346-354Article in journal (Refereed)
    Abstract [en]

    An O-acetyl-4-O methylglucuronoxylan-rich wood hydrolysate (WH), generated by the hydrothermal treatment of hardwood, was chain extended using di- and tri-functionalized amino chain extenders through reductive amination. Chain extension was achieved via facile one- or two-step syntheses. The carbohydrate chain extension efficiency, molecular weights, and branching patterns were determined through a combination of SEC, 1HNMR, FUR and elemental analysis. The mild reaction conditions enabled an increase in the molecular weight while preserving the initial structures of the hemicelluloses. The chain extension strategy developed in this study was demonstrated to significantly improve the formability and mechanical performance of WH films, allowing for the water-casting production of coherent films with higher ratios of WH - 70-85% (w/w) - and reducing the need for co-components. Chain-extended WHs produced stronger and more ductile films than corresponding formulations prepared from unmodified WH. Films made from ethylenediamine chain-extended WH mixed with 30% (w/w) carboxymethyl cellulose showed a tensile strength of 62 MPa and a strain-to-failure of 3.3%. Additionally, chain-extended WHs produced films with an oxygen permeability as low as 0.2 cm(3) mu M m(-2) day(-1) kPa(-1) at 50% RH.

  • 6.
    Ibn Yaich, Anas
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology.
    Edlund, Ulrica
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
    Albertsson, Ann-Christine
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
    Transfer of Biomatrix/Wood Cell Interactions to Hemicellulose-Based Materials to Control Water Interaction2017In: Chemical Reviews, ISSN 0009-2665, E-ISSN 1520-6890, Vol. 117, no 12, p. 8177-8207Article, review/survey (Refereed)
    Abstract [en]

    The family of hemicelluloses stands out as a very promising natural resource that can be utilized as a biobased materials feedstock. An in-depth understanding of the hemicellulose inherent structural and property features as well as the structure property relationships induced by the specific supramolecular hierarchical organization of lignocellulosic biopolymers will be a key enabling technology in the emerging biorefinery sector. This Review aims to give a perspective on these issues and demonstrate how the transfer of molecular wood cell interactions into hemicellulose-based materials may offer new design principles for material formulations.

  • 7.
    Ibn Yaich, Anas
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology.
    Edlund, Ulrica
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology.
    Albertsson, Ann-Christine
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology.
    Wood Hydrolysate Barriers: Performance Controlled via Selective Recovery2012In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 13, no 2, p. 466-473Article in journal (Refereed)
    Abstract [en]

    Films and coatings were produced from a noncellulosic polysaccaride-rich wood hydrolysate (WH) and the resulting oxygen barrier performance was improved by a selective choice of upgrading conditions. The WH was obtained from process water in the hydrothermal treatment of hardwood and subjected to one of three alternative upgrading treatments, resulting in xylan-rich fractions with significant differences in structure, composition, and properties of the recovered WH fractions, which in turn had a major impact on their performance with respect to tensile and oxygen barrier properties. The WH in the least upgraded state, the crudest fraction, produced films with the best performance in terms of oxygen permeability and was superior to corresponding films based on highly purified hemicellulose.

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