| 1. |
- Ciftci, Göksu Cinar, et al.
(författare)
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Tailoring of rheological properties and structural polydispersity effects in microfibrillated cellulose suspensions
- 2020
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Ingår i: Cellulose. - : Springer Science+Business Media B.V.. - 0969-0239 .- 1572-882X. ; 27:16, s. 9227-9241
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Tidskriftsartikel (refereegranskat)abstract
- Abstract: Industrial production of low-charge microfibrillated cellulose (MFC) typically results in wide fibril size distributions. This polydispersity influences viscosity, overall colloidal stability, and rheological properties of MFC suspensions and gels in aqueous systems. In this work, a systematic rheological analysis is performed for industrially prepared MFC and fractions of different size distributions. Gel formation and flow characteristics (e.g., shear-thinning) of each fraction are examined under neutral and acidic conditions and compared with the unfractionated MFC suspension. The effects of size, aspect ratio, and surface charge on the rheology of semi-dilute MFC suspensions are discussed. The results demonstrate that particle size and aspect ratio distribution control the viscoelasticity and shear-thinning properties of MFC suspensions. An increased fraction of small diameter nanofibrils, by ex situ addition of the fine particles with high aspect ratio or removal of the coarsest particles (with lower aspect ratio) by fractionation, significantly enhances the storage modulus and the yield stress of the complex mixture, compared to the properties of the coarser fractions. New insights are also reported on the tailoring of the rheology of highly polydisperse fibrillar mixtures, where the rheological contributions of each fraction are discussed. Graphic abstract: [Figure not available: see fulltext.].
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| 2. |
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| 3. |
- Li, Lengwan, et al.
(författare)
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Ultrastrong Ionotronic Films Showing Electrochemical Osmotic Actuation
- 2023
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Ingår i: Advanced Materials. - : Wiley. - 0935-9648 .- 1521-4095. ; 35:45
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Tidskriftsartikel (refereegranskat)abstract
- A multifunctional soft material with high ionic and electrical conductivity, combined with high mechanical properties and the ability to change shape can enable bioinspired responsive devices and systems. The incorporation of all these characteristics in a single material is very challenging, as the improvement of one property tends to reduce other properties. Here, a nanocomposite film based on charged, high-aspect-ratio 1D flexible nanocellulose fibrils, and 2D Ti3C2Tx MXene is presented. The self-assembly process results in a stratified structure with the nanoparticles aligned in-plane, providing high ionotronic conductivity and mechanical strength, as well as large water uptake. In hydrogel form with 20 wt% liquid, the electrical conductivity is over 200 S cm−1 and the in-plane tensile strength is close to 100 MPa. This multifunctional performance results from the uniquely layered composite structure at nano- and mesoscales. A new type of electrical soft actuator is assembled where voltage as low as ±1 V resulted in osmotic effects and giant reversible out-of-plane swelling, reaching 85% strain.
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| 4. |
- Walther, Andreas, et al.
(författare)
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Best Practice for Reporting Wet Mechanical Properties of Nanocellulose-Based Materials
- 2020
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Ingår i: Biomacromolecules. - : American Chemical Society (ACS). - 1525-7797 .- 1526-4602. ; 21:6, s. 2536-2540
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Tidskriftsartikel (refereegranskat)abstract
- Nanocellulose-based materials and nanocomposites show extraordinary mechanical properties with high stiffness, strength, and toughness. Although the last decade has witnessed great progress in understanding the mechanical properties of these materials, a crucial challenge is to identify pathways to introduce high wet strength, which is a critical parameter for commercial applications. Because of the waterborne fabrication methods, nanocellulose-based materials are prone to swelling by both adsorption of moist air or liquid water. Unfortunately, there is currently no best practice on how to take the swelling into account when reporting mechanical properties at different relative humidity or when measuring the mechanical properties of fully hydrated materials. This limits and in parts fully prevents comparisons between different studies. We review current approaches and propose a best practice for measuring and reporting mechanical properties of wet nanocellulose-based materials, highlighting the importance of swelling and the correlation between mechanical properties and volume expansion.
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| 5. |
- Wohlert, Malin, et al.
(författare)
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Cellulose and the role of hydrogen bonds : not in charge of everything
- 2022
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Ingår i: Cellulose. - : Springer Nature. - 0969-0239 .- 1572-882X. ; 29:1, s. 1-23
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Tidskriftsartikel (refereegranskat)abstract
- In the cellulose scientific community, hydrogen bonding is often used as the explanation for a large variety of phenomena and properties related to cellulose and cellulose based materials. Yet, hydrogen bonding is just one of several molecular interactions and furthermore is both relatively weak and sensitive to the environment. In this review we present a comprehensive examination of the scientific literature in the area, with focus on theory and molecular simulation, and conclude that the relative importance of hydrogen bonding has been, and still is, frequently exaggerated.
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| 6. |
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| 7. |
- Castro, Daniele Oliveira, et al.
(författare)
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The use of a pilot-scale continuous paper process for fire retardant cellulose-kaolinite nanocomposites
- 2018
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Ingår i: Composites Science And Technology. - : Elsevier Ltd. - 0266-3538 .- 1879-1050. ; 162, s. 215-224
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Tidskriftsartikel (refereegranskat)abstract
- Nanostructured materials are difficult to prepare rapidly and at large scale. Melt-processed polymer-clay nanocomposites are an exception, but the clay content is typically below 5 wt%. An approach for manufacturing of microfibrillated cellulose (MFC)/kaolinite nanocomposites is here demonstrated in pilot-scale by continuous production of hybrid nanopaper structures with thickness of around 100 μm. The colloidal nature of MFC suspensions disintegrated from chemical wood fiber pulp offers the possibility to add kaolinite clay platelet particles of nanoscale thickness. For initial lab scale optimization purposes, nanocomposite processing (dewatering, small particle retention etc) and characterization (mechanical properties, density etc) were investigated using a sheet former (Rapid Köthen). This was followed by a continuous fabrication of composite paper structures using a pilot-scale web former. Nanocomposite morphology was assessed by scanning electron microscopy (SEM). Mechanical properties were measured in uniaxial tension. The fire retardancy was evaluated by cone calorimetry. Inorganic hybrid composites with high content of in-plane oriented nanocellulose, nanoclay and wood fibers were successfully produced at pilot scale. Potential applications include fire retardant paperboard for semi structural applications and as reinforcement mats in molded thermoset biocomposites.
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| 8. |
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| 9. |
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| 10. |
- Farahani, Saina Kishani, et al.
(författare)
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Experimental and Theoretical Evaluation of the Solubility/Insolubility of Spruce Xylan (Arabino Glucuronoxylan)
- 2019
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Ingår i: Biomacromolecules. - : American Chemical Society (ACS). - 1525-7797 .- 1526-4602. ; 20:3, s. 1263-1270
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Tidskriftsartikel (refereegranskat)abstract
- © 2019 American Chemical Society. The molecular solubility of softwood arabinoglucuronoxylan (AGX) has been thoroughly investigated, and it has been shown that the chemical and physical structures of the extracted hemicellulose are not significantly influenced by different purification steps, but a transient molecular solubility of AGX was observed in aqueous media at low concentrations (1 g/L) when the dissolved macromolecules had a hydrodynamic diameter of up to 10 nm. A phase separation was detected when the concentration was increased to 15 g/L leading to an association of the smaller molecules into fractal structures with a considerably larger diameter, even though the dispersions were still transparent to ocular inspection. Dynamic Light Scattering and Cryo-Transmission Electron Microscopy showed dimensions in the range of 1000 nm. The phase separation of the sample was further characterized by estimating the χ-interaction parameter of AGX in water using the Flory-Huggins theory, and the results supported that water is a poor solvent for AGX. This behavior is crucial when films and hydrogels based on these biopolymers are made, since the association will dramatically affect barrier and mechanical properties of films made from these materials.
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| 11. |
- Francon, Hugo, et al.
(författare)
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Ambient-Dried, 3D-Printable and Electrically Conducting Cellulose Nanofiber Aerogels by Inclusion of Functional Polymers
- 2020
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Ingår i: Advanced Functional Materials. - : Wiley-VCH Verlag. - 1616-301X .- 1616-3028.
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Tidskriftsartikel (refereegranskat)abstract
- This study presents a novel, green, and efficient way of preparing crosslinked aerogels from cellulose nanofibers (CNFs) and alginate using non-covalent chemistry. This new process can ultimately facilitate the fast, continuous, and large-scale production of porous, light-weight materials as it does not require freeze-drying, supercritical CO2 drying, or any environmentally harmful crosslinking chemistries. The reported preparation procedure relies solely on the successive freezing, solvent-exchange, and ambient drying of composite CNF-alginate gels. The presented findings suggest that a highly-porous structure can be preserved throughout the process by simply controlling the ionic strength of the gel. Aerogels with tunable densities (23–38 kg m−3) and compressive moduli (97–275 kPa) can be prepared by using different CNF concentrations. These low-density networks have a unique combination of formability (using molding or 3D-printing) and wet-stability (when ion exchanged to calcium ions). To demonstrate their use in advanced wet applications, the printed aerogels are functionalized with very high loadings of conducting poly(3,4-ethylenedioxythiophene):tosylate (PEDOT:TOS) polymer by using a novel in situ polymerization approach. In-depth material characterization reveals that these aerogels have the potential to be used in not only energy storage applications (specific capacitance of 78 F g−1), but also as mechanical-strain and humidity sensors. © 2020 The Authors.
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| 12. |
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| 13. |
- Karim, Zoheb, et al.
(författare)
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Forming a cellulose based nanopaper using XPM
- 2017
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Ingår i: International Conference on Nanotechnology for Renewable Materials 2017. - : TAPPI Press. - 9781510850897 ; , s. 399-407
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Konferensbidrag (refereegranskat)
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| 14. |
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| 15. |
- Larsson, Per A., 1980-, et al.
(författare)
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Towards optimised size distribution in commercial microfibrillated cellulose : a fractionation approach
- 2019
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Ingår i: Cellulose. - : Springer. - 0969-0239 .- 1572-882X. ; 26:3, s. 1565-1575
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Tidskriftsartikel (refereegranskat)abstract
- For the successful commercialisation of microfibrillated cellulose (MFC) it is of utmost importance to carefully characterise the constituent cellulose particles. This could for instance lead to the development of MFC grades with size distributions tailored for specific applications. Characterization of MFC is challenging due to the heterogeneous chemical and structural nature of MFC. This study describes a fractionation approach that combines two steps of physical sieving of larger particles and a final centrifugation step to separate out the smallest, colloidally stable particles, resulting in four distinctly different size fractions. The properties, such as size and charge, of each fraction were studied, as well as MFC filtration time, film formation, and film properties (mechanical and optical). It was found that virtually all surface charges, determined by polyelectrolyte adsorption, are located in the colloidally stable fraction of the MFC. In addition, the amount of available surface charges can be used as an estimate of the degree of fibrillation of the MFC. The partly fibrillated particles frequently displayed a branching, fringed morphology. Mechanical testing of films from the different fractions revealed that the removal of large particles may be more important for strength than achieving full fibrillation. Overall, this study demonstrates that by controlling the size distribution in MFC grades, property profiles including dewatering time to make films by filtration, rheology, film strength and optical transmittance could be optimised. [GRAPHICS] .
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| 16. |
- Nordenström, Malin
(författare)
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Colloidal interactions and arrested dynamics of cellulose nanofibrils
- 2020
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Over the past decades, concerns for the environment have increased and efforts to achieve a sustainable society have intensified. One particular challenge is to replace fossil-based plastics with biodegradable materials produced from renewable resources. Cellulose nanofibril (CNF)-based materials are strong candidates due to their excellent mechanical properties, nano-dimensions and molecular structure, which is suitable for modification. CNFs can be obtained from wood and are elongated, often charged, particles which are usually handled in aqueous dispersions. The colloidal stability is sensitive, and instability results in aggregation or transition to an arrested state. Since the properties of CNF-based materials rely on dispersion of the CNFs, an understanding of the colloidal behaviour is crucial.This work has focused on the interactions and dynamics of CNFs in different colloidal states. Arrested states of CNFs were studied in detail and it was found that two types of arrested state exist, with different colloidal interactions and mechanisms governing their formation. The dynamics in arrested and dispersed states were studied by tracer diffusion measurements, and it was found that small amounts of CNFs can constitute an excellent stabiliser for other particle dispersions according to a so far unexplored mechanism.The effects of altering the colloidal interactions using different strategies were also evaluated. The counterions of CNFs were exchanged and the impact on the swelling behaviour was measured. Based on the results, different contributions to the counterion-dependent interactions are discussed. Two strategies for using polymers to alter the interactions were furthermore studied. Polyethylene glycol (PEG) was grafted to CNFs in order to increase the arrested state threshold concentration. PEG, carboxymethyl cellulose and lignin, were also used as additives which improved the redispersion of dried CNF, especially in the case of samples containing lignin.
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| 17. |
- Nordenström, Malin, et al.
(författare)
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Colloidal interactions in nanocellulose systems
- 2016
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Ingår i: Abstracts of Papers of the American Chemical Society. - : AMER CHEMICAL SOC. - 0065-7727. ; 251
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Tidskriftsartikel (övrigt vetenskapligt/konstnärligt)
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| 18. |
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| 19. |
- Senf, Deborah, et al.
(författare)
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Tailormade Polysaccharides with Defined Branching Patterns: Enzymatic Polymerization of Arabinoxylan Oligosaccharides
- 2018
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Ingår i: Angewandte Chemie - International Edition. - : Wiley. - 1433-7851 .- 1521-3773. ; 57:37, s. 11987-11992
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Tidskriftsartikel (refereegranskat)abstract
- The heterogeneous nature of non-cellulosic polysaccharides, such as arabinoxylan, makes it difficult to correlate molecular structure with macroscopic properties. To study the impact of specific structural features of the polysaccharides on crystallinity or affinity to other cell wall components, collections of polysaccharides with defined repeating units are required. Herein, a chemoenzymatic approach to artificial arabinoxylan polysaccharides with systematically altered branching patterns is described. The polysaccharides were obtained by glycosynthase-catalyzed polymerization of glycosyl fluorides derived from arabinoxylan oligosaccharides. X-ray diffraction and adsorption experiments on cellulosic surfaces revealed that the physicochemical properties of the synthetic polysaccharides strongly depend on the specific nature of their substitution patterns. The artificial polysaccharides allow structure–property relationship studies that are not accessible by other means.
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| 20. |
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| 21. |
- Alipoormazandarani, Niloofar, et al.
(författare)
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Functional Lignin Nanoparticles with Tunable Size and Surface Properties : Fabrication, Characterization, and Use in Layer-by-Layer Assembly
- 2021
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 13:22, s. 26308-26317
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Tidskriftsartikel (refereegranskat)abstract
- Lignin is the richest source of renewable aromatics and has immense potential for replacing synthetic chemicals. The limited functionality of lignin is, however, challenging for its potential use, which motivates research for creating advanced functional lignin-derived materials. Here, we present an aqueous-based acid precipitation method for preparing functional lignin nanoparticles (LNPs) from carboxy-methylated or carboxy-pentylated lignin. We observe that the longer grafted side chains of carboxy-pentylated lignin allow for the formation of larger LNPs. The functional nanoparticles have high tolerance against salt and aging time and well-controlled size distribution with R-h <= 60 nm over a pH range of 5-11. We further investigate the layer-by-layer (LbL) assembly of the LNPs and poly(allylamine hydrochloride) (PAH) using a stagnation point adsorption reflectometry (SPAR) and quartz crystal microbalance with dissipation (QCM-D). Results demonstrate that LNPs made of carboxypentylated lignin (i.e., PLNPs with the adsorbed mass of 3.02 mg/m(2)) form a more packed and thicker adlayer onto the PAH surface compared to those made of carboxymethylated lignin (i.e., CLNPs with the adsorbed mass of 2.51 mg/m(2)). The theoretical flux, J, and initial rate of adsorption, (d Gamma/dt)(0), analyses confirm that 22% of PLNPs and 20% of CLNPs arriving at the PAH surface are adsorbed. The present study provides a feasible platform for engineering LNPs with a tunable size and adsorption behavior, which can be adapted in hionanomaterial production.
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| 22. |
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| 23. |
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| 24. |
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| 25. |
- Arumughan, Vishnu, 1994, et al.
(författare)
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Specific ion effects in the adsorption of carboxymethyl cellulose on cellulose: The influence of industrially relevant divalent cations
- 2021
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Ingår i: Colloids and Surfaces A: Physicochemical and Engineering Aspects. - : Elsevier BV. - 1873-4359 .- 0927-7757. ; 626
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Tidskriftsartikel (refereegranskat)abstract
- The adsorption of carboxymethylcellulose (CMC) on cellulose surfaces is of relevance from both academic and industrial perspectives as it facilitates resource-efficient modification of cellulose fibres that allows them to carry negative charges. It is known that, compared to monovalent ions, Ca2+ ions are superior ions in facilitating CMC adsorption and the subsequent introduction of charge on cellulose fibres. However, the formation and deposition of calcium oxide involved in this process necessitates the search for alternative cations. Magnesium ions form one of the more promising candidates since they are already used in the pulping process to prevent cellulose degradation during peroxide bleaching. This work aims at elucidating the effects of the industrially relevant alkaline earth metal divalent cations Mg2+ and Ca2+ on the CMC adsorption process onto cellulose surfaces. Quartz Crystal Microbalance (QCM-D) technology was used to follow the adsorption in model systems in real time, whereas the adsorption of CMC on commercial fibres was studied using polyelectrolyte titrations, total organic carbon (TOC) analysis and conductometric titrations. This study shows that the presence of Ca2+ ions was more favourable for the adsorption of CMC to both types of cellulosic surfaces than Mg2+ ions. The distinction in the adsorption behaviour in the presence of Mg2+ and Ca2+ is suggested to be due to the differences in the polarizability of the ions. The findings are decisive in designing efficient industrial processes for the adsorption of polyelectrolytes to cellulose surfaces of similar charge.
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| 26. |
- Asta, Nadia
(författare)
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Fundamentals of Interactions between Cellulose Materials and its Implications on Properties of Fibrous Networks
- 2024
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Fundamental research plays a pivotal role in the development of sustainable solutions that benefit both our environment and everyday lives. Cellulose, as an abundant and renewable resource, holds immense potential for sustainable applications. However, navigating the complexities of molecular and supramolecular structure of cellulose poses significant challenges in harnessing its full potential. By delving into fundamental research, we aim to uncover the underlying mechanisms governing cellulose interactions, paving the way for innovative advancements in sustainable material development.This thesis uncovers the intricate relationship between fundamental research and applied methodologies by showing how molecular contact and structure at the interface of cellulose-rich materials will control the development of the macroscopic mechanical properties of networks from cellulose-rich fibres. The study encompasses various facets, ranging from the development of model materials for studying interfacial interactions to the preparation of fibrous networks with tailored properties.In the initial part of the work the research delves into the development of model materials to investigate interactions at smooth interfaces of regenerated cellulose. The study reveals the crucial role of the making and breaking of cellulose interface, or sometimes interphase, in the development of adhesive joints. Experimental findings demonstrate how chemical additives influence the interactions between cellulose surfaces, thereby modulating the structural and adhesive properties at the interface. Furthermore, by utilizing model materials, insights are gained into fibre-fibre interactions and the influence of surface treatments on network formation and mechanical performance. Lastly, the research focused on investigating the preparation of fibrous networks at different densities and amount of adsorbed additives, providing a comprehensive understanding of how network density and composition affect mechanical properties of the networks.This work not only exemplifies a synergistic approach, where fundamental insights into molecular contacts and interface structures are translated into practical applications for enhancing macroscopic properties but also highlights the importance of integrating fundamental and applied methodologies in molecular engineering, offering novel strategies for advancing sustainable paper production practices and contributing to the attainment of sustainable development goals.
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| 27. |
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| 28. |
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| 29. |
- Asta, Nadia, et al.
(författare)
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The Use of Model Cellulose Materials for Studying Molecular Interactions at Cellulose Interfaces
- 2023
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Ingår i: ACS Macro Letters. - : American Chemical Society (ACS). - 2161-1653. ; 12, s. 1530-1535
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 30. |
- Atoufi Najafabadi, Zhaleh
(författare)
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Development and Tailoring of Low‐Density Cellulose‐Based Structures for Water Treatment
- 2024
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The challenges posed by our limited clean water sources and the well-known global water pollution demand more efficient water purification technologies. Additionally, the increasing environmental awareness has inspired a shift towards eco-friendly and renewable materials and technologies. This thesis is focused on developing effective adsorbent materials from renewable resources to eliminate organic solvents, dyes, and metal ions from water. Cellulose, the most abundant biopolymer in nature, is the main component used to develop new materials in the present study. Its distinctive physical and colloidal properties, in the form of nanocellulose, along with tunable surface chemistry, play key roles in enhancing the effectiveness of the developed materials.The primary focus of the first part of the thesis was to develop a molecular layer-by-layer modification technique to customize the surface functionality of cellulose aerogels in a uniform and controlled manner. Through the sequential deposition of diamine and triacid monomers, exceeding lythin polyamide coatings were formed on the cellulose aerogels, altering the surface properties from hydrophilic to hydrophobic. This transformation made them well-suited structures for oil-water separation.Following this, a biohybrid aerogel was developed based on cellulose nanofibrils (CNFs) and amyloid nanofibrils (ANFs), the latter derived by heat treatment of β-lactoglobulin proteins. The pH-tunable surface charge of the aerogel, controlled by the amphiphilicity of the protein, allowed for the adsorption of both cationic and anionic contaminants by adjusting the pH of the solutions. Furthermore, the aerogels exhibited remarkable selectivity for lead (II) ions and they could also be regenerated and reused after each adsorption cycle without a significant loss of their adsorption capacity. This was to a large extent possible due to the excellent wet stability of these aerogels, which was achieved by crosslinking the CNFs during freezing and ice templating, eliminating the need for freeze-drying. However, a solvent exchange to acetone after melting was still necessary to reduce the influence of the capillary forces during drying to avoid the collapse of the aerogels. In a consecutive study, the foaming characteristics of the heat-treated β-lactoglobulin system were exploited to create highly stable Pickering foams with the aid of using CNFs as stabilizers and to physically lock the system through a controlled pH reduction. Interestingly, these Pickering foams could be directly oven-dried without collapsing, yielding low-density foams. Furthermore, it was demonstrated that the foams can be chemically crosslinked by incorporating chemical crosslinkers in the formulation or by pre-functionalizing the CNFs with dialdehydes. This crosslinking naturally also provided wet stability to the oven-dried foams.Finally, an innovative and environmentally friendly method was introduced to increase the charge of cellulose fibers by radical polymerization of acrylic acid from the fibers, enabling the preparation of fibers with an exceptionally high charge of 6.7 mmol/g. The introduction of these charged groups significantly enhanced the interaction of the fibers with methylene blue as a model dye and lead (II), Copper (II), and Zinc (II) ions as model metal ions, showing the huge potential of these fibers as building blocks for a wide range of adsorbent applications. Overall, this thesis demonstrates the development and characterization of several bio-based adsorbents for water remediation.
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| 31. |
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| 32. |
- Atoufi, Zhaleh, et al.
(författare)
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Green Ambient-Dried Aerogels with a Facile pH-Tunable Surface Charge for Adsorption of Cationic and Anionic Contaminants with High Selectivity
- 2022
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Ingår i: Biomacromolecules. - : American Chemical Society (ACS). - 1525-7797 .- 1526-4602. ; 23:11, s. 4934-4947
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Tidskriftsartikel (refereegranskat)abstract
- The fabrication of reusable, sustainable adsorbents from low-cost, renewable resources via energy efficient methods is challenging. This paper presents wet-stable, carboxymethylated cellulose nanofibril (CNF) and amyloid nanofibril (ANF) based aerogel-like adsorbents prepared through efficient and green processes for the removal of metal ions and dyes from water. The aerogels exhibit tunable densities (18-28 kg m-3), wet resilience, and an interconnected porous structure (99% porosity), with a pH controllable surface charge for adsorption of both cationic (methylene blue and Pb(II)) and anionic (brilliant blue, congo red, and Cr(VI)) model contaminants. The Langmuir saturation adsorption capacity of the aerogel was calculated to be 68, 79, and 42 mg g-1for brilliant blue, Pb(II), and Cr(VI), respectively. Adsorption kinetic studies for the adsorption of brilliant blue as a model contaminant demonstrated that a pseudo-second-order model best fitted the experimental data and that an intraparticle diffusion model suggests that there are three adsorption stages in the adsorption of brilliant blue on the aerogel. Following three cycles of adsorption and regeneration, the aerogels maintained nearly 97 and 96% of their adsorption capacity for methylene blue and Pb(II) as cationic contaminants and 89 and 80% for brilliant blue and Cr(VI) as anionic contaminants. Moreover, the aerogels showed remarkable selectivity for Pb(II) in the presence of calcium and magnesium as background ions, with a selectivity coefficient more than 2 orders of magnitude higher than calcium and magnesium. Overall, the energy-efficient and sustainable fabrication procedure, along with good structural stability, reusability, and selectivity, makes these aerogels very promising for water purification applications.
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| 33. |
- Atoufi, Zhaleh, et al.
(författare)
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Surface tailoring of cellulose aerogel-like structures with ultrathin coatings using molecular layer-by-layer assembly
- 2022
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Ingår i: Carbohydrate Polymers. - : Elsevier BV. - 0144-8617 .- 1879-1344. ; 282
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Tidskriftsartikel (refereegranskat)abstract
- Cellulose nanofibril-based aerogels have promising applicability in various fields; however, developing an effi-cient technique to functionalize and tune their surface properties is challenging. In this study, physically and covalently crosslinked cellulose nanofibril-based aerogel-like structures were prepared and modified by a mo-lecular layer-by-layer (m-LBL) deposition method. Following three m-LBL depositions, an ultrathin polyamide layer was formed throughout the aerogel and its structure and chemical composition was studied in detail. Analysis of model cellulose surfaces showed that the thickness of the deposited layer after three m-LBLs was approximately 1 nm. Although the deposited layer was extremely thin, it led to a 2.6-fold increase in the wet specific modulus, improved the acid-base resistance, and changed the aerogels from hydrophilic to hydrophobic making them suitable materials for oil absorption with the absorption capacity of 16-36 g/g. Thus, demon-strating m-LBL assembly is a powerful technique for tailoring surface properties and functionality of cellulose substrates.
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| 34. |
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| 35. |
- Atoufi, Zhaleh, et al.
(författare)
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Synergistically stabilized wet foams from heat treated β-lactoglobulin and cellulose nanofibrils and their application for green foam production
- 2024
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Ingår i: Applied Materials Today. - : Elsevier BV. - 2352-9407. ; 39
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Tidskriftsartikel (refereegranskat)abstract
- Achieving a sustainable foam production requires a complete substitution of synthetic components with natural and renewable alternatives, as well as development of an environment-friendly production process. This work demonstrates a synergetic combination of heat-treated beta-lactoglobulin proteins and cellulose nanofibrils (CNFs) to create fully bio-based and highly-stable wet foams. Furthermore, a gradual reduction in the pH, enabled oven-drying of the wet foams without any major structural collapse of the foam, resulting in the preparation of lightweight solid foams with the density of 10.2 kg.m(-3). First, the foaming behavior of heat-treated beta-lactoglobulin systems (HBSs) containing amyloid nanofibrils (ANFs) and non-converted peptides was investigated at different pHs. Subsequently, the HBS foams were stabilized using CNFs, followed by a gradual acidification of the system to a final pH of 4.5. To gain a deeper understanding of the stabilization mechanism of the foam, the interactions between the foam's components, their positioning in the foam structure, and the viscoelasticity of the fibrillar network were investigated using quartz crystal microgravimetry, confocal microscopy and rheology. The analysis of the obtained data suggests that the stability of the foams was associated with the accumulation of CNFs and ANFs at the air-water interface, and that the concomitant formation of an intertwined network surrounding the air bubbles. This together resulted in a significant decrease in drainage rate of the liquid in the foam lamellae, bubble coarsening and bubble coalescence within the foams. The results also show that the major surface-active component participating in the creation of the foam is the free peptide left in solution after the formation of the ANFs. A slow reduction in pH to 4.5 lead to further gelation of the fibrillar network and an improved storage modulus of the foam lamellae. This resulted in a strong coherent structure that could withstand oven-drying without collapse. The density, porosity, microstructure and compressive mechanical properties of such prepared dry foams were assessed. Overall, the results demonstrate the potential of HBSs to replace synthetic surfactants and outlines a sustainable preparation protocol for the preparation of light-weight porous composite structures of ANFs and CNFs.
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| 36. |
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| 37. |
- Aulin, Christian, 1980-, et al.
(författare)
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Buildup of polyelectrolyte multilayers of polyethyleneimine and microfibrillated cellulose studied by in situ dual-polarization interferometry and quartz crystal microbalance with dissipation
- 2008
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Ingår i: Langmuir. - : American Chemical Society (ACS). - 0743-7463 .- 1520-5827. ; 24:6, s. 2509-2518
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Tidskriftsartikel (refereegranskat)abstract
- Polyethyleneimine (PEI) and Microfibrillated cellulose (MFC) have been used to buildup polyelectrolyte multilayers (PEM) on silicone oxide and silicone oxynitride surfaces at different pH values and with different electrolyte and polyelectrolyte/colloid concentrations of the components. Consecutive adsorption on these surfaces was studied by in situ dual-polarization interferometry (DPI) and quartz crystal microbalance measurements. The adsorption data obtained from both the techniques showed a steady buildup of multilayers. High pH and electrolyte concentration of the PEI solution was found to be beneficial for achieving a high adsorbed amount of PEI, and hence of MFC, during the buildup of the multilayer. On the other hand, an increase in the electrolyte concentration of the MFC dispersion was found to inhibit the adsorption of MFC onto PEL The adsorbed amount of MFC was independent of the bulk MFC concentration in the investigated concentration range (15-250 mg/L). Atomic force microscopy measurements were used to image a MFC-treated silicone oxynitride chip from DPI measurements. The surface was found to be almost fully covered by randomly oriented microfibrils after the adsorption of only one bilayer of PEI/MFC. The surface roughness expressed as the rms-roughness over 1 ÎŒm2 was calculated to be 4.6 nm (1 bilayer). The adsorbed amount of PEI and MFC and the amount of water entrapped by the individual layers in the multilayer structures were estimated by combining results from the two analytical techniques using the de Feijter formula. These results indicate a total water content of ca. 41% in the PEM.
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| 38. |
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| 39. |
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| 40. |
- Belaineh, Dagmawi, et al.
(författare)
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Controlling the Organization of PEDOT:PSS on Cellulose Structures
- 2019
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Ingår i: ACS APPLIED POLYMER MATERIALS. - : AMER CHEMICAL SOC. - 2637-6105. ; 1:9, s. 2342-2351
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Tidskriftsartikel (refereegranskat)abstract
- Composites of biopolymers and conducting polymers are emerging as promising candidates for a green technological future and are actively being explored in various applications, such as in energy storage, bioelectronics, and thermoelectrics. While the device characteristics of these composites have been actively investigated, there is limited knowledge concerning the fundamental intracomponent interactions and the modes of molecular structuring. Here, by use of cellulose and poly(3,4-ethylene-dioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), it is shown that the chemical and structural makeup of the surfaces of the composite components are critical factors that determine the materials organization at relevant dimensions. AFM, TEM, and GIVVAXS measurements show that when mixed with cellulose nanofibrils, PEDOT:PSS organizes into continuous nanosized beadlike structures with an average diameter of 13 nm on the nanofibrils. In contrast, when PEDOT:PSS is blended with molecular cellulose, a phase-segregated conducting network morphology is reached, with a distinctly relatively lower electric conductivity. These results provide insight into the mechanisms of PEDOT:PSS crystallization and may have significant implications for the design of conducting biopolymer composites for a vast array of applications.
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| 41. |
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| 42. |
- Benselfelt, Tobias, et al.
(författare)
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Electrochemically Controlled Hydrogels with Electrotunable Permeability and Uniaxial Actuation
- 2023
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Ingår i: Advanced Materials. - : Wiley. - 0935-9648 .- 1521-4095. ; 35:45
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Tidskriftsartikel (refereegranskat)abstract
- The unique properties of hydrogels enable the design of life-like soft intelligent systems. However, stimuli-responsive hydrogels still suffer from limited actuation control. Direct electronic control of electronically conductive hydrogels can solve this challenge and allow direct integration with modern electronic systems. An electrochemically controlled nanowire composite hydrogel with high in-plane conductivity that stimulates a uniaxial electrochemical osmotic expansion is demonstrated. This materials system allows precisely controlled shape-morphing at only −1 V, where capacitive charging of the hydrogel bulk leads to a large uniaxial expansion of up to 300%, caused by the ingress of ≈700 water molecules per electron–ion pair. The material retains its state when turned off, which is ideal for electrotunable membranes as the inherent coupling between the expansion and mesoporosity enables electronic control of permeability for adaptive separation, fractionation, and distribution. Used as electrochemical osmotic hydrogel actuators, they achieve an electroactive pressure of up to 0.7 MPa (1.4 MPa vs dry) and a work density of ≈150 kJ m−3 (2 MJ m−3 vs dry). This new materials system paves the way to integrate actuation, sensing, and controlled permeation into advanced soft intelligent systems.
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| 43. |
- Benselfelt, Tobias, et al.
(författare)
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Explaining the Exceptional Wet Integrity of Transparent Cellulose Nanofibril Films in the Presence of Multivalent Ions-Suitable Substrates for Biointerfaces
- 2019
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Ingår i: Advanced Materials Interfaces. - : WILEY. - 2196-7350. ; 6:13
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Tidskriftsartikel (refereegranskat)abstract
- Cellulose nanofibrils (CNFs) assemble into water-resilient materials in the presence of multivalent counter-ions. The essential mechanisms behind these assemblies are ion-ion correlation and specific ion effects. A network model shows that the interfibril attraction indirectly influences the wet modulus by a fourth power relationship to the solidity of the network (E-w proportional to phi(4)). Ions that induce both ion-ion correlation and specific ion effects significantly reduce the swelling of the films, and due to the nonlinear relationship dramatically increase the wet modulus. Herein, this network model is used to explain the elastoplastic behavior of wet films of 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO)-oxidized, carboxymethylated, and phosphorylated CNFs in the presence of different counter-ions. The main findings are that the aspect ratio of the CNFs influences the ductility of the assemblies, that the bivalency of phosphorylate ligands probably limits the formation of interfibril complexes with divalent ions, and that a higher charge density increases the friction between fibrils by increasing the short-range attraction from ion-ion correlation and specific ion effects. These findings can be used to rationally design CNF materials for a variety of applications where wet strength, ductility, and transparency are important, such as biomaterials or substrates for bioelectronics.
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| 44. |
- Benselfelt, Tobias, et al.
(författare)
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Ion-induced assemblies of highly anisotropic nanoparticles are governed by ion-ion correlation and specific ion effects
- 2019
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Ingår i: Nanoscale. - : Royal Society of Chemistry. - 2040-3364 .- 2040-3372. ; 11:8, s. 3514-3520
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Tidskriftsartikel (refereegranskat)abstract
- Ion-induced assemblies of highly anisotropic nanoparticles can be explained by a model consisting of ion-ion correlation and specific ion effects: dispersion interactions, metal-ligand complexes, and local acidic environments. Films of cellulose nanofibrils and montmorillonite clay were treated with different ions, and their subsequent equilibrium swelling in water was related to important parameters of the model in order to investigate the relative importance of the mechanisms. Ion-ion correlation was shown to be the fundamental attraction, supplemented by dispersion interaction for polarizable ions such as Ca2+ and Ba2+, or metal-ligand complexes for ions such as Cu2+, Al3+ and Fe3+. Ions that form strong complexes induce local acidic environments that also contribute to the assembly. These findings are summarized in a comprehensive semi-quantitative model and are important for the design of nanomaterials and for understanding biological systems where specific ions are involved.
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| 45. |
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| 46. |
- Benselfelt, Tobias, et al.
(författare)
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Supramolecular double networks of cellulose nanofibrils and algal polysaccharides with excellent wet mechanical properties
- 2018
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Ingår i: Green Chemistry. - : ROYAL SOC CHEMISTRY. - 1463-9262 .- 1463-9270. ; 20:11, s. 2558-2570
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Tidskriftsartikel (refereegranskat)abstract
- Supramolecular double network films, consisting of cellulose nanofibrils (CNF) entangled with the algal polysaccharides alginate or carrageenan, were prepared using a rapid vacuum filtration process to achieve water-resistant CNF nanopapers with excellent mechanical properties in both the wet and dry states following the locking of the structures using Ca2+. The rigid network of calcium alginate was more efficient than the more flexible network of calcium carrageenan and 10% by weight of alginate was sufficient to form a network that suppressed the swelling of the CNF film by over 95%. The resulting material could be compared to a stiff rubber with a Young's modulus of 135 MPa, a tensile strength of 17 MPa, a strain-at-break above 55%, and a work of fracture close to 5 MJ m(-3) in the wet state, which was both significantly stronger and more ductile than the calcium-treated CNF reference nanopaper. It was shown that the state in which Ca2+ was introduced is crucial, and it is also hypothesized that the alginate works as a sacrificial network that prevents the CNF from aligning during loading and that this leads to the increased toughness. The material maintained its barrier properties at elevated relative humidities and the extensibility and ductility made possible hygroplastic forming into three-dimensional shapes. It is suggested that the attractive force in the CNF part of the double network in the presence of multivalent ions is due to the ion-ion correlation forces generated by the fluctuating counter-ion cloud, since no significant ion coordination was observed using FTIR.
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| 47. |
- Benselfelt, Tobias, et al.
(författare)
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The Colloidal Properties of Nanocellulose
- 2023
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Ingår i: ChemSusChem. - : John Wiley and Sons Inc. - 1864-5631 .- 1864-564X. ; 16:8, s. e202201955-
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Tidskriftsartikel (refereegranskat)abstract
- Nanocelluloses are anisotropic nanoparticles of semicrystalline assemblies of glucan polymers. They have great potential as renewable building blocks in the materials platform of a more sustainable society. As a result, the research on nanocellulose has grown exponentially over the last decades. To fully utilize the properties of nanocelluloses, a fundamental understanding of their colloidal behavior is necessary. As elongated particles with dimensions in a critical nanosize range, their colloidal properties are complex, with several behaviors not covered by classical theories. In this comprehensive Review, we describe the most prominent colloidal behaviors of nanocellulose by combining experimental data and theoretical descriptions. We discuss the preparation and characterization of nanocellulose dispersions, how they form networks at low concentrations, how classical theories cannot describe their behavior, and how they interact with other colloids. We then show examples of how scientists can use this fundamental knowledge to control the assembly of nanocellulose into new materials with exceptional properties. We hope aspiring and established researchers will use this Review as a guide. © 2023 The Authors.
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| 48. |
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| 49. |
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| 50. |
- Bosmans, Toon, 1988, et al.
(författare)
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Assembly of Debranched Xylan from Solution and on Nanocellulosic Surfaces
- 2014
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Ingår i: Biomacromolecules. - : American Chemical Society (ACS). - 1525-7797 .- 1526-4602. ; 15:3, s. 924-930
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Tidskriftsartikel (refereegranskat)abstract
- This study focused on the assembly characteristics of debranched xylan onto cellulose surfaces. A rye arabinoxylan polymer with an initial arabinose/xylose ratio of 0.53 was debranched with an oxalic acid treatment as a function of time. The resulting samples contained reduced arabinose/xylose ratios significantly affecting the molecular architecture and solution behavior of the biopolymer. With this treatment, an almost linear xylan with arabinose DS of only 0.04 was obtained. The removal of arabinose units resulted in the self-assembly of the debranched polymer in water into stable nanoparticle aggregates with a size around 300 nm with a gradual increase in crystallinity of the isolated xylan. Using quartz crystal microbalance with dissipation monitoring, the adsorption of xylan onto model cellulose surfaces was quantified. Compared to the nonmodified xylan, the adsorption of debranched xylan increased from 0.6 to 5.5 mg m(-2). Additionally, adsorption kinetics suggest that the nanoparticles rapidly adsorbed to the cellulose surfaces compared to the arabinoxylan. In summary, a control of the molecular structure of xylan influences its ability to form a new class of polysaccharide nanoparticles in aqueous suspensions and its interaction with nanocellulose surfaces.
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