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  • 1.
    Abbadessa, Anna
    et al.
    KTH Royal institute of Technology, Sweden.
    Dogaris, Ioannis
    KTH Royal institute of Technology, Sweden.
    Kishani Farahani, Saina
    KTH Royal institute of Technology, Sweden.
    Reid, Michael S.
    KTH Royal institute of Technology, Sweden.
    Rautkoski, Hille
    VTT Technical Research Centre of Finland, Finland.
    Holopainen-Mantila, Ulla
    VTT Technical Research Centre of Finland, Finland.
    Oinonen, Petri
    Ecohelix, Sweden.
    Henriksson, Gunnar
    KTH Royal institute of Technology, Sweden.
    Layer-by-layer assembly of sustainable lignin-based coatings for food packaging applications2023In: Progress in organic coatings, ISSN 0300-9440, E-ISSN 1873-331X, Vol. 182, article id 107676Article in journal (Refereed)
    Abstract [en]

    Packaging plays a critical role in ensuring food safety and shelf life by protecting against e.g., moisture, gases, and light. Polyethylene (PE) is widely used in food packaging, but it is mainly produced from non-renewable resources and it is an inefficient oxygen and light barrier. In this study, the layer-by-layer (LbL) assembly of a sustainably produced lignin-based polymer (EH) with polyethylenimine (PEI) or chitosan (CH) was used to fabricate (partially or fully) bio-based coatings with the aim of improving barrier properties of PE films. The charge density of EH was calculated using a polyelectrolyte titration method and the hydrodynamic diameters of EH, PEI and CH were determined by Dynamic Light Scattering (DLS). LbL assembly was monitored in situ via Quartz Crystal Microbalance with Dissipation (QCM-D) and Stagnation Point Adsorption Reflectometry (SPAR). PE films were coated with a variable number of PEI/EH or CH/EH bilayers (BL) using an immersive LbL assembly method. Coated films were studied in terms of light-blocking ability, wettability, thermal behaviour, surface structure, as well as oxygen and water vapor barrier properties. QCM-D and SPAR data showed a stepwise multilayer formation and strong interactions between the oppositely charged polymers, with PEI/EH coating having a greater amount of deposited polymer compared to CH/EH coating at the same number of BL. Overall, light barrier properties and wettability of the coated films increased with the number of deposited bilayers. Coated PE films maintained the overall thermal behaviour of PE. A number of BL of 20 was found to be the most promising based on the studied properties. Selected samples showed improved oxygen and water vapor barrier properties, with PEI/EH coating performing better than CH/EH coating. Taken altogether, we demonstrated that a novel and sustainable lignin-based polymer can be combined with PEI or CH to fabricate (partially or fully) bio-based coatings for food packaging. 

  • 2.
    Asta, Nadia
    et al.
    KTH Royal institute of Technology, Sweden.
    Reid, Michael S.
    RISE Research Institutes of Sweden, Bioeconomy and Health, Material and Surface Design. KTH Royal institute of Technology, Sweden.
    Pettersson, Torbjörn
    KTH Royal institute of Technology, Sweden.
    Wågberg, Lars
    KTH Royal institute of Technology, Sweden.
    The Use of Model Cellulose Materials for Studying Molecular Interactions at Cellulose Interfaces2023In: ACS Macro Letters, E-ISSN 2161-1653, Vol. 12, p. 1530-1535Article in journal (Refereed)
    Abstract [en]

    Despite extensive research on biobased and fiber-based materials, fundamental questions regarding the molecular processes governing fiber-fiber interactions remain unanswered. In this study, we introduce a method to examine and clarify molecular interactions within fiber-fiber joints using precisely characterized model materials, i.e., regenerated cellulose gel beads with nanometer-smooth surfaces. By physically modifying these materials and drying them together to create model joints, we can investigate the mechanisms responsible for joining cellulose surfaces and how this affects adhesion in both dry and wet states through precise separation measurements. The findings reveal a subtle balance in the joint formation, influencing the development of nanometer-sized structures at the contact zone and likely inducing built-in stresses in the interphase. This research illustrates how model materials can be tailored to control interactions between cellulose-rich surfaces, laying the groundwork for future high-resolution studies aimed at creating stiff, ductile, and/or tough joints between cellulose surfaces and to allow for the design of high-performance biobased materials. 

  • 3.
    Attias, Noam
    et al.
    Israel Institute of Technology, Israel.
    Reid, Michael
    KTH Royal Institute of Technology, Sweden.
    Mijowska, Sylwia
    Israel Institute of Technology, Israel.
    Dobryden, Illia
    KTH Royal Institute of Technology, Sweden.
    Isaksson, Marcus
    RISE Research Institutes of Sweden.
    Pokroy, Boaz
    Israel Institute of Technology, Israel.
    Grobman, Yasha
    Israel Institute of Technology, Israel.
    Abitbol, Tiffany
    RISE Research Institutes of Sweden, Bioeconomy and Health, Material and Surface Design.
    Biofabrication of Nanocellulose–Mycelium Hybrid Materials2021In: Advanced Sustainable Systems, ISSN 2366-7486, Vol. 5, no 2, article id 2000196Article in journal (Refereed)
    Abstract [en]

    Healthy material alternatives based on renewable resources and sustainable technologies have the potential to disrupt the environmentally damaging production and consumption practices established throughout the modern industrial era. In this study, a mycelium–nanocellulose biocomposite with hybrid properties is produced by the agitated liquid culture of a white-rot fungus (Trametes ochracea) with nanocellulose (NC) comprised as part of the culture media. Mycelial development proceeds via the formation of pellets, where NC is enriched in the pellets and depleted from the surrounding liquid media. Micrometer-scale NC elements become engulfed in mycelium, whereas it is hypothesized that the nanometer-scale fraction becomes integrated within the hyphal cell wall, such that all NC in the system is essentially surface-modified by mycelium. The NC confers mechanical strength to films processed from the biocomposite, whereas the mycelium screens typical cellulose–water interactions, giving fibrous slurries that dewater faster and films that exhibit significantly improved wet resistance in comparison to pure NC films. The mycelium–nanocellulose biocomposites are processable in the ways familiar to papermaking and are suggested for diverse applications, including packaging, filtration, and hygiene products.

  • 4.
    Gorur, Yunus
    et al.
    KTH Royal Institute of Technology, Sweden.
    Reid, Michael
    KTH Royal Institute of Technology, Sweden.
    Montanari, Celine
    KTH Royal Institute of Technology, Sweden; Wallenberg Wood Science Center, Sweden.
    Larsson, Per Tomas
    RISE Research Institutes of Sweden. KTH Royal Institute of Technology, Sweden.
    Larsson, Per A.
    KTH Royal Institute of Technology, Sweden.
    Wågberg, Lars
    KTH Royal Institute of Technology, Sweden.
    Advanced Characterization of Self-Fibrillating Cellulose Fibers and Their Use in Tunable Filters2021In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 13, no 27, p. 32467-32478Article in journal (Refereed)
    Abstract [en]

    Thorough characterization and fundamental understanding of cellulose fibers can help us develop new, sustainable material streams and advanced functional materials. As an emerging nanomaterial, cellulose nanofibrils (CNFs) have high specific surface area and good mechanical properties; however, handling and processing challenges have limited their widespread use. This work reports an in-depth characterization of self-fibrillating cellulose fibers (SFFs) and their use in smart, responsive filters capable of regulating flow and retaining nanoscale particles. By combining direct and indirect characterization methods with polyelectrolyte swelling theories, it was shown that introduction of charges and decreased supramolecular order in the fiber wall were responsible for the exceptional swelling and nanofibrillation of SFFs. Different microscopy techniques were used to visualize the swelling of SFFs before, during, and after nanofibrillation. Through filtration and pH adjustment, smart filters prepared via in situ nanofibrillation showed an ability to regulate the flow rate through the filter and a capacity of retaining 95% of 300 nm (diameter) silica nanoparticles. This exceptionally rapid and efficient approach for making smart filters directly addresses the challenges associated with dewatering of CNFs and bridges the gap between science and technology, making the widespread use of CNFs in high-performance materials a not-so-distant reality. 

  • 5.
    Reid, Michael
    et al.
    KTH Royal Institute of Technology, Sweden.
    Karlsson, Maria
    RISE Research Institutes of Sweden. Linköping University, Sweden.
    Abitbol, Tiffany
    RISE Research Institutes of Sweden, Bioeconomy and Health, Material and Surface Design.
    Fluorescently labeled cellulose nanofibrils for detection and loss analysis2020In: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 250, article id 116943Article in journal (Refereed)
    Abstract [en]

    Fluorescently labeled cellulose nanofibrils (CNFs) were used to evaluate CNF leaching from paper according to standard safety assays for food contact materials. Enzymatically pretreated pulp was first labeled with 5-([4,6-Dichlorotriazin-2-yl]amino)fluorescein hydrochloride (DTAF), followed by homogenization to produce fluorescent CNFs of varying degrees of fibrillation. Labeling at the μmolar DTAF/g cellulose level imparted quantitative ppb fluorescence detection of CNFs (LOD of approximately 20 ppb), without significantly altering other material properties, suggesting that DTAF-labeled CNFs are an appropriate mimic for native CNFs and that this approach can be used to detect low CNF concentrations. Cold and hot-water extractions of laboratory papers (100 % CNFs and CNF-fiber blended papers) showed loss values below 3 wt% CNFs, with the finest CNF quality showing the least loss overall and with greater loss experienced under hot water conditions compared with cold water. DTAF-labeled CNFs can be used to address questions related to CNF distribution, localization, and loss. 

  • 6.
    Reid, Michael S.
    et al.
    RISE Research Institutes of Sweden, Bioeconomy and Health, Material and Surface Design. The Digital Cellulose Center, Sweden.
    Suganda, Widi
    KTH Royal institute of Technology, Sweden.
    Östmark, Emma
    Stora Enso, Sweden.
    Brolin, Anders
    Stora Enso, Sweden.
    Wågberg, Lars
    KTH Royal institute of Technology, Sweden.
    Dewatering of Micro- and Nanofibrillated Cellulose for Membrane Production2023In: ACS Sustainable Chemistry and Engineering, E-ISSN 2168-0485, Vol. 11, p. 16428-41Article in journal (Refereed)
    Abstract [en]

    Cellulose-based membranes have tremendous potential to improve the sustainability and performance of high value applications, such as filters and energy devices, particularly as fluorinated compounds are becoming more regulated. Yet, a deeper understanding of how cellulose films are formed and their structure, in both the wet and dry state, is needed to meet application specific demands and scale-up. We investigated cellulose dewatering using dead-end filtration and the effect of particle size, pressure, temperature, ionic strength, and pH were explored. Dewatering times, filtration cake resistance and compressibility of microfibrillated celluloses (MFCs) and cellulose nanofibrils (CNFs), (and a combination thereof) were measured to understand the role of fibrillation and intermolecular forces during dewatering and forming of membranes. In this fundamental work, dewatering behavior was well described by conventional filtration theory and increasing the pressure from 1 to 4 bar reduced dewatering times by one-half with no significant impact on the mechanical properties. Cake compressibility was found to be directly related to particle size and degree of fibrillation, indicating that finer grades of MFCs and CNFs could be more effectively dewatered at higher pressures. Adjusting pH and ionic strength of cellulose dispersions could similarly reduce dewatering times, yet impacted the wet and dry mechanical properties. This work serves as a basis to better understand the structure-property relationships that develop during dewatering of MFCs and CNFs. 

  • 7.
    Sethi, Jatin
    et al.
    KTH Royal Institute of Technology, Sweden.
    Glowacki, Eric
    Linköping University, Sweden; Brno University of Technology, Czech Republic.
    Reid, Michael
    RISE Research Institutes of Sweden, Bioeconomy and Health, Material and Surface Design. KTH Royal Institute of Technology, Sweden.
    Larsson, Per A.
    KTH Royal Institute of Technology, Sweden.
    Wågberg, Lars
    KTH Royal Institute of Technology, Sweden.
    Ultra-thin parylene-aluminium hybrid coatings on nanocellulose films to resist water sensitivity2024In: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 323, article id 121365Article in journal (Refereed)
    Abstract [en]

    Non-sustainable single-use plastics used for food packaging needs to be phased out. Films made from cellulose nanofibrils (CNFs) are suitable candidates for biodegradable and recyclable packaging materials as they exhibit good mechanical properties, excellent oxygen barrier properties and high transparency. Yet, their poor water vapour barrier properties have been a major hindrance in their commercialisation. Here, we describe the preparation of 25 μm thick CNF films with significantly improved water vapour barrier properties after deposition of ultrathin polymeric and metallic coatings, parylene C and aluminium, respectively. When first adding a 40 nm aluminium layer followed by an 80 nm parylene layer, i.e. with a combined thickness of less than one percent of the CNF film, a water vapour transmission rate of 2.8 g m−2 d−1 was achieved at 38 °C and 90 % RH, surpassing a 25 μm polypropylene film (4–12 g m−2 d−1). This is an improvement of more than 700 times compared to uncoated CNF films, under some of the harshest possible conditions a packaging material will need to endure in commercial use. The layers showed a good and even coverage, as assessed by atomic force microscopy, and the parylene-coated surfaces were hydrophobic with a contact angle of 110°, providing good water repellency. 

  • 8.
    Yang, Xuan
    et al.
    KTH Royal Institute of Technology, Sweden; Zhejiang University, China.
    Li, Lengwan
    KTH Royal Institute of Technology, Sweden.
    Nishiyama, Yohiharu
    Universite Grenoble Alpes, France.
    Reid, Michael
    RISE Research Institutes of Sweden, Bioeconomy and Health, Material and Surface Design. KTH Royal Institute of Technology, Sweden.
    Berglund, Lars A
    KTH Royal Institute of Technology, Sweden.
    Processing strategy for reduced energy demand of nanostructured CNF/clay composites with tailored interfaces2023In: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 312, article id 120788Article in journal (Refereed)
    Abstract [en]

    Nacre-mimicking nanocomposites based on colloidal cellulose nanofibrils (CNFs) and clay nanoparticles show excellent mechanical properties, yet processing typically involves preparation of two colloids followed by a mixing step, which is time- and energy-consuming. In this study, a facile preparation method using low energy kitchen blenders is reported in which CNF disintegration, clay exfoliation and mixing carried out in one step. Compared to composites made from the conventional method, the energy demand is reduced by about 97 %; the composites also show higher strength and work to fracture. Colloidal stability, CNF/clay nanostructure, and CNF/clay orientation are well characterized. The results suggest favorable effects from hemicellulose-rich, negatively charged pulp fibers and corresponding CNFs. CNF disintegration and colloidal stability are facilitated with substantial CNF/clay interfacial interaction. The results show a more sustainable and industrially relevant processing concept for strong CNF/clay nanocomposites. © 2023 The Authors

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