| 1. |
- Görür, Yunus Can, et al.
(författare)
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Advanced Characterization of Self-Fibrillating Cellulose Fibers and Their Use in Tunable Filters
- 2021
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society. - 1944-8244 .- 1944-8252. ; 13:27, s. 32467-32478
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 2. |
- Rosén, Tomas, 1985-, et al.
(författare)
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Cross-Sections of Nanocellulose from Wood Analyzed by Quantized Polydispersity of Elementary Microfibrils
- 2020
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Ingår i: ACS Nano. - : American Chemical Society. - 1936-0851 .- 1936-086X. ; 14:12, s. 16743-16754
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Tidskriftsartikel (refereegranskat)abstract
- Bio-based nanocellulose has been shown to possess impressive mechanical properties and simplicity for chemical modifications. The chemical properties are largely influenced by the surface area and functionality of the nanoscale materials. However, finding the typical cross-sections of nanocellulose, such as cellulose nanofibers (CNFs), has been a long-standing puzzle, where subtle changes in extraction methods seem to yield different shapes and dimensions. Here, we extracted CNFs from wood with two different oxidation methods and variations in degree of oxidation and high-pressure homogenization. The cross-sections of CNFs were characterized by small-angle X-ray scattering and wide-angle X-ray diffraction in dispersed and freeze-dried states, respectively, where the results were analyzed by assuming that the cross-sectional distribution was quantized with an 18-chain elementary microfibril, the building block of the cell wall. We find that the results agree well with a pseudosquare unit having a size of about 2.4 nm regardless of sample, while the aggregate level strongly depends on the extraction conditions. Furthermore, we find that aggregates have a preferred cohesion of phase boundaries parallel to the (110)-plane of the cellulose fibril, leading to a ribbon shape on average.
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| 3. |
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| 4. |
- Elf, Patric, et al.
(författare)
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Molecular Dynamics Simulations of Cellulose and Dialcohol Cellulose under Dry and Moist Conditions
- 2023
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Ingår i: Biomacromolecules. - : American Chemical Society (ACS). - 1525-7797 .- 1526-4602. ; 24:6, s. 2706-2720
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Tidskriftsartikel (refereegranskat)abstract
- The development of wood-based thermoplastic polymers that can replace synthetic plastics is of high environmental importance, and previous studies have indicated that cellulose-rich fiber containing dialcohol cellulose (ring-opened cellulose) is a very promising candidate material. In this study, molecular dynamics simulations, complemented with experiments, were used to investigate how and why the degree of ring opening influences the properties of dialcohol cellulose, and how temperature and presence of water affect the material properties. Mechanical tensile properties, diffusion/mobility-related properties, densities, glass-transition temperatures, potential energies, hydrogen bonds, and free volumes were simulated for amorphous cellulosic materials with 0-100% ring opening, at ambient and high (150 °C) temperatures, with and without water. The simulations showed that the impact of ring openings, with respect to providing molecular mobility, was higher at high temperatures. This was also observed experimentally. Hence, the ring opening had the strongest beneficial effect on “processability” (reduced stiffness and strength) above the glass-transition temperature and in wet conditions. It also had the effect of lowering the glass-transition temperature. The results here showed that molecular dynamics is a valuable tool in the development of wood-based materials with optimal thermoplastic properties.
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| 5. |
- Kotov, Nikolay, et al.
(författare)
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Elucidating the fine-scale structural morphology of nanocellulose by nano infrared spectroscopy
- 2023
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Ingår i: Carbohydrate Polymers. - : Elsevier Ltd. - 0144-8617 .- 1879-1344. ; 302
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Tidskriftsartikel (refereegranskat)abstract
- Nanoscale infrared (IR) spectroscopy and microscopy, enabling the acquisition of IR spectra and images with a lateral resolution of 20 nm, is employed to chemically characterize individual cellulose nanocrystals (CNCs) and cellulose nanofibrils (CNFs) to elucidate if the CNCs and CNFs consist of alternating crystalline and amorphous domains along the CNF/CNC. The high lateral resolution enables studies of the nanoscale morphology at different domains of the CNFs/CNCs: flat segments, kinks, twisted areas, and end points. The types of nanocellulose investigated are CNFs from tunicate, CNCs from cotton, and anionic and cationic wood-derived CNFs. All nano-FTIR spectra acquired from the different samples and different domains of the individual nanocellulose particles resemble a spectrum of crystalline cellulose, suggesting that the non-crystalline cellulose signal observed in macroscopic measurements of nanocellulose most likely originate from cellulose chains present at the surface of the nanocellulose particles.
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| 6. |
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| 7. |
- Rostami, Jowan, et al.
(författare)
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Hierarchical build-up of bio-based nanofibrous materials with tunable metal-organic framework biofunctionality
- 2021
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Ingår i: Materials Today. - : Elsevier BV. - 1369-7021 .- 1873-4103. ; 48, s. 47-58
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Tidskriftsartikel (refereegranskat)abstract
- Multifunctional, light-weight, responsive materials show promise in a range of applications including soft robotics, therapeutic delivery, advanced diagnostics and charge storage. This paper presents a novel, scalable, efficient and sustainable approach for the preparation of cellulose nanofibril-based aerogels via a facile ice-templating, solvent exchange and air-drying procedure, which could replace existing inefficient drying processes. These ambient-dried aerogels (similar to 99% porosity) exhibit a high specific compressive modulus (26.8 +/- 6.1 kPa m(3) kg(-1), approaching equivalence of carbon-nanotubereinforced aerogels), wet stability and shape recovery (80-90%), favorable specific surface area (90 m(2) g(-1)) and tunable densities (2-20 kg m(-3)). The aerogels provide an ideal nanofibrillar substrate for in-situ growth of metal-organic frameworks (MOFs), via co-assembly of MOF precursors with proteins in aqueous solutions. The resulting hybrid aerogels show a nine-fold increase in surface area (810 m(2)g(-1)), with preserved wet stability and additional protein biofunctionality. The hybrid aerogels facilitate a pH-controlled release of immobilized proteins, following a concomitant disassembly of the surface grown MOFs, demonstrating their use in controlled delivery systems. The colorimetric protein binding assay of the biofunctionalized hybrid aerogel also demonstrates the potential of the material as a novel 3D bioassay platform, which could potentially be an alternative to plate-based enzyme-linked immunosorbent assay.
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| 8. |
- Thomas, Richard D., et al.
(författare)
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The double electrostatic ion ring experiment : A unique cryogenic electrostatic storage ring for merged ion-beams studies
- 2011
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Ingår i: Review of Scientific Instruments. - : AIP Publishing. - 0034-6748 .- 1089-7623. ; 82:6, s. 065112-
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Tidskriftsartikel (refereegranskat)abstract
- We describe the design of a novel type of storage device currently under construction at Stockholm University, Sweden, using purely electrostatic focussing and deflection elements, in which ion beams of opposite charges are confined under extreme high vacuum cryogenic conditions in separate rings and merged over a common straight section. The construction of this double electrostatic ion ring experiment uniquely allows for studies of interactions between cations and anions at low and well-defined internal temperatures and centre-of-mass collision energies down to about 10 K and 10 meV, respectively. Position sensitive multi-hit detector systems have been extensively tested and proven to work in cryogenic environments and these will be used to measure correlations between reaction products in, for example, electron-transfer processes. The technical advantages of using purely electrostatic ion storage devices over magnetic ones are many, but the most relevant are: electrostatic elements which are more compact and easier to construct; remanent fields, hysteresis, and eddy-currents, which are of concern in magnetic devices, are no longer relevant; and electrical fields required to control the orbit of the ions are not only much easier to create and control than the corresponding magnetic fields, they also set no upper mass limit on the ions that can be stored. These technical differences are a boon to new areas of fundamental experimental research, not only in atomic and molecular physics but also in the boundaries of these fields with chemistry and biology. For examples, studies of interactions with internally cold molecular ions will be particular useful for applications in astrophysics, while studies of solvated ionic clusters will be of relevance to aeronomy and biology.
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| 9. |
- 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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| 10. |
- 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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