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Östmans, R., Benselfelt, T., Erlandsson, J., Rostami, J., Hall, S., Lindström, S. B. & Wågberg, L. (2024). Solidified water at room temperature hosting tailored fluidic channels by using highly anisotropic cellulose nanofibrils. Materials Today Nano, 26, Article ID 100476.
Open this publication in new window or tab >>Solidified water at room temperature hosting tailored fluidic channels by using highly anisotropic cellulose nanofibrils
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2024 (English)In: Materials Today Nano, E-ISSN 2588-8420, Vol. 26, article id 100476Article in journal (Refereed) Published
Abstract [en]

Highly anisotropic cellulose nanofibrils can solidify liquid water, creating self-supporting structures by incorporating a tiny number of fibrils. These fibrillar hydrogels can contain as much as 99.99 wt% water. The structure and mechanical properties of fibrillar networks have so far not been completely understood, nor how they solidify the bulk water at such low particle concentrations. In this work, the mechanical properties of cellulose fibrillar hydrogels in the dilute regime from a wt% perspective have been studied, and an elastoplastic model describing the network structure and its mechanics is presented. A significant insight from this work is that the ability of the fibrils to solidify water is very dependent on particle stiffness and the number of contact points it can form in the network structure. The comparison between the experimental results and the theoretical model shows that the fibrillar networks in the dilute regime form via a non-stochastic process since the fibrils have the time and freedom to find contact points during network formation by translational and rotational diffusion. The formed, dilute fibrillar network deforms by sliding fibril contacts upon straining the network beyond its elastic limit. Our results also show that before macroscopic failure, the fibril contacts are restored once the load is released. The exceptional properties of this solidified water are exploited to host fluidic channels, allowing directed fluid transportation in water. Finally, the microfluidic channels formed in the hydrogels are tailored by the layer-by-layer technique to be interactive against external stimuli, a characteristic envisioned to be useful in biomedical applications.

Place, publisher, year, edition, pages
Elsevier BV, 2024
Keywords
Cellulose nanofibrils, Channels, Colloidal gel, Fibrillar hydrogels, Layer-by-layer, Network model
National Category
Materials Engineering
Identifiers
urn:nbn:se:kth:diva-345750 (URN)10.1016/j.mtnano.2024.100476 (DOI)2-s2.0-85189942008 (Scopus ID)
Note

QC 20240424

Available from: 2024-04-18 Created: 2024-04-18 Last updated: 2024-04-29Bibliographically approved
Wang, Z., Heasman, P., Rostami, J., Benselfelt, T., Linares, M., Li, H., . . . Wågberg, L. (2023). Dynamic Networks of Cellulose Nanofibrils Enable Highly Conductive and Strong Polymer Gel Electrolytes for Lithium-Ion Batteries. Advanced Functional Materials, 33(30), Article ID 2212806.
Open this publication in new window or tab >>Dynamic Networks of Cellulose Nanofibrils Enable Highly Conductive and Strong Polymer Gel Electrolytes for Lithium-Ion Batteries
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2023 (English)In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 33, no 30, article id 2212806Article in journal (Refereed) Published
Abstract [en]

Tunable dynamic networks of cellulose nanofibrils (CNFs) are utilized to prepare high-performance polymer gel electrolytes. By swelling an anisotropically dewatered, but never dried, CNF gel in acidic salt solutions, a highly sparse network is constructed with a fraction of CNFs as low as 0.9%, taking advantage of the very high aspect ratio and the ultra-thin thickness of the CNFs (micrometers long and 2–4 nm thick). These CNF networks expose high interfacial areas and can accommodate massive amounts of the ionic conductive liquid polyethylene glycol-based electrolyte into strong homogeneous gel electrolytes. In addition to the reinforced mechanical properties, the presence of the CNFs simultaneously enhances the ionic conductivity due to their excellent strong water-binding capacity according to computational simulations. This strategy renders the electrolyte a room-temperature ionic conductivity of 0.61 ± 0.12 mS cm−1 which is one of the highest among polymer gel electrolytes. The electrolyte shows superior performances as a separator for lithium iron phosphate half-cells in high specific capacity (161 mAh g−1 at 0.1C), excellent rate capability (5C), and cycling stability (94% capacity retention after 300 cycles at 1C) at 60 °C, as well as stable room temperature cycling performance and considerably improved safety compared with commercial liquid electrolyte systems.

Place, publisher, year, edition, pages
Wiley, 2023
Keywords
cellulose nanofibrils, composites, energy storages, lithium-ion batteries, polymer electrolytes
National Category
Materials Chemistry Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-338472 (URN)10.1002/adfm.202212806 (DOI)000973324900001 ()2-s2.0-85152801974 (Scopus ID)
Note

QC 20231115

Available from: 2023-11-15 Created: 2023-11-15 Last updated: 2023-11-15Bibliographically approved
Östmans, R., Cortes Ruiz, M. F., Rostami, J., Sellman, F. A., Wågberg, L., Lindström, S. B. & Benselfelt, T. (2023). Elastoplastic behavior of anisotropic, physically crosslinked hydrogel networks comprising stiff, charged fibrils in an electrolyte. Soft Matter, 19(15), 2792-2800
Open this publication in new window or tab >>Elastoplastic behavior of anisotropic, physically crosslinked hydrogel networks comprising stiff, charged fibrils in an electrolyte
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2023 (English)In: Soft Matter, ISSN 1744-683X, E-ISSN 1744-6848, Vol. 19, no 15, p. 2792-2800Article in journal (Refereed) Published
Abstract [en]

Fibrillar hydrogels are remarkably stiff, low-density networks that can hold vast amounts of water. These hydrogels can easily be made anisotropic by orienting the fibrils using different methods. Unlike the detailed and established descriptions of polymer gels, there is no coherent theoretical framework describing the elastoplastic behavior of fibrillar gels, especially concerning anisotropy. In this work, the swelling pressures of anisotropic fibrillar hydrogels made from cellulose nanofibrils were measured in the direction perpendicular to the fibril alignment. This experimental data was used to develop a model comprising three mechanical elements representing the network and the osmotic pressure due to non-ionic and ionic surface groups on the fibrils. At low solidity, the stiffness of the hydrogels was dominated by the ionic swelling pressure governed by the osmotic ingress of water. Fibrils with different functionality show the influence of aspect ratio, chemical functionality, and the remaining amount of hemicelluloses. This general model describes physically crosslinked hydrogels comprising fibrils with high flexural rigidity - that is, with a persistence length larger than the mesh size. The experimental technique is a framework to study and understand the importance of fibrillar networks for the evolution of multicellular organisms, like plants, and the influence of different components in plant cell walls.

Place, publisher, year, edition, pages
Royal Society of Chemistry (RSC), 2023
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-330921 (URN)10.1039/d2sm01571d (DOI)000960684700001 ()36992628 (PubMedID)2-s2.0-85152114916 (Scopus ID)
Note

QC 20230704

Available from: 2023-07-04 Created: 2023-07-04 Last updated: 2024-04-29Bibliographically approved
Sellman, F. A., Benselfelt, T., Larsson, P. T. & Wågberg, L. (2023). Hornification of cellulose-rich materials: A kinetically trapped state. Carbohydrate Polymers, 318, Article ID 121132.
Open this publication in new window or tab >>Hornification of cellulose-rich materials: A kinetically trapped state
2023 (English)In: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 318, article id 121132Article in journal (Refereed) Published
Abstract [en]

The fundamental understanding concerning cellulose-cellulose interactions under wet and dry conditions remains unclear. This is especially true regarding the drying-induced association of cellulose, commonly described as an irreversible phenomenon called hornification. A fundamental understanding of the mechanisms behind hornification would contribute to new drying techniques for cellulose-based materials in the pulp and paper industry while at the same time enhancing material properties and facilitating the recyclability of cellulose-rich materials. In the present work, the irreversible joining of cellulose-rich surfaces has been studied by subjecting cellulose nanofibril (CNF) films to different heat treatments to establish a link between reswelling properties, structural characteristics as well as chemical and mechanical analyses. A heating time/temperature dependence was observed for the reswelling of the CNF films, which is related to the extent of hornification and is different for different chemical compositions of the fibrils. Further, the results indicate that hornification is related to a diffusion process and that the reswellability increases very slowly over long time, indicating that equilibrium is not reached. Hence, hornification is suggested to be a kinetically limited phenomenon governed by non-covalent reversible interactions and a time/temperature dependence on their forming and breaking.

Place, publisher, year, edition, pages
Elsevier BV, 2023
Keywords
Aggregation, Cellulose nanofibril, Hornification, Kinetics, Swelling
National Category
Materials Chemistry Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-334855 (URN)10.1016/j.carbpol.2023.121132 (DOI)001056626000001 ()37479442 (PubMedID)2-s2.0-85163374088 (Scopus ID)
Note

QC 20230829

Available from: 2023-08-28 Created: 2023-08-28 Last updated: 2024-05-07Bibliographically approved
Alexakis, A. E., Telaretti Leggieri, R., Wågberg, L., Malmström, E. & Benselfelt, T. (2023). Nanolatex architectonics: Influence of cationic charge density and size on their adsorption onto surfaces with a 2D or 3D distribution of anionic groups. Journal of Colloid and Interface Science, 634, 610-620
Open this publication in new window or tab >>Nanolatex architectonics: Influence of cationic charge density and size on their adsorption onto surfaces with a 2D or 3D distribution of anionic groups
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2023 (English)In: Journal of Colloid and Interface Science, ISSN 0021-9797, E-ISSN 1095-7103, Vol. 634, p. 610-620Article in journal (Refereed) Published
Place, publisher, year, edition, pages
Elsevier BV, 2023
National Category
Chemical Sciences Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-324121 (URN)10.1016/j.jcis.2022.12.038 (DOI)000960700700001 ()36549209 (PubMedID)2-s2.0-85144465921 (Scopus ID)
Funder
Knut and Alice Wallenberg Foundation
Note

QC 20230426

Available from: 2023-02-21 Created: 2023-02-21 Last updated: 2023-04-26Bibliographically approved
Benselfelt, T., Kummer, N., Nordenström, M., Fall, A. B., Nyström, G. & Wågberg, L. (2023). The Colloidal Properties of Nanocellulose. ChemSusChem, 16(8), Article ID e202201955.
Open this publication in new window or tab >>The Colloidal Properties of Nanocellulose
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2023 (English)In: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564X, ChemSusChem, ISSN 1864-5631, Vol. 16, no 8, article id e202201955Article, review/survey (Refereed) Published
Abstract [en]

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.

Place, publisher, year, edition, pages
Wiley, 2023
Keywords
aspect ratio, assembly, colloidal interactions, nanocellulose, networks
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-332984 (URN)10.1002/cssc.202201955 (DOI)000940357600001 ()36650954 (PubMedID)2-s2.0-85149045814 (Scopus ID)
Note

QC 20230724

Available from: 2023-07-24 Created: 2023-07-24 Last updated: 2023-07-24Bibliographically approved
Wohlert, M., Benselfelt, T., Wågberg, L., Furo, I., Berglund, L. & Wohlert, J. (2022). Cellulose and the role of hydrogen bonds: not in charge of everything. Cellulose, 29(1), 1-23
Open this publication in new window or tab >>Cellulose and the role of hydrogen bonds: not in charge of everything
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2022 (English)In: Cellulose, ISSN 0969-0239, E-ISSN 1572-882X, Vol. 29, no 1, p. 1-23Article in journal (Refereed) Published
Abstract [en]

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.

Place, publisher, year, edition, pages
Springer Nature, 2022
Keywords
Cellulose, Computer modeling, Hydrogen bonding, Nanomaterials, Hydrogen bonds, Molecular structure, Cellulose based materials, Comprehensive examination, Computer models, Molecular simulations, Phenomena and properties, Scientific community, Scientific literature, Documents, Examination, Materials
National Category
Information Systems, Social aspects
Identifiers
urn:nbn:se:kth:diva-313261 (URN)10.1007/s10570-021-04325-4 (DOI)000720243800001 ()2-s2.0-85119261613 (Scopus ID)
Note

QC 20220608

Available from: 2022-06-08 Created: 2022-06-08 Last updated: 2022-06-25Bibliographically approved
Alexakis, A. E., Jerlhagen, Å., Telaretti Leggieri, R., Eliasson, A., Benselfelt, T. & Malmström, E. (2022). Modification of CNF‐Networks by the Addition of Small Amounts of Well‐Defined Rigid Cationic Nanolatexes. Macromolecular Chemistry and Physics, 224(1), 2200249-2200249
Open this publication in new window or tab >>Modification of CNF‐Networks by the Addition of Small Amounts of Well‐Defined Rigid Cationic Nanolatexes
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2022 (English)In: Macromolecular Chemistry and Physics, ISSN 1022-1352, E-ISSN 1521-3935, Vol. 224, no 1, p. 2200249-2200249Article in journal (Refereed) Published
Abstract [en]

Cellulose nanofibril (CNF)-networks are modified by the addition of small amounts (below 10 wt%) of well-defined cationic nanolatexes synthesized through reversible addition–fragmentation chain-transfer-mediated polymerization-induced self-assembly (PISA). Minute amounts of nanolatex inclusions lead to increased tensile and shear moduli, indicating that nanolatexes can act as bridging-points between CNFs. At higher nanolatex content, this stiffening effect is lost, likely due to interactions between nanolatexes leading to plasticization. The influence of nanolatex content and size on interparticle distance is discussed and is used as a tool to understand the effects observed in macroscopic properties. Upon annealing, the stiffening effect is lost due to the softening of the nanolatexes, indicating that the core–shell morphology is a prerequisite for this effect. These systems form a versatile platform to develop fundamental insights into complex condensed colloidal systems, to ultimately aid in the development of new sustainable material concepts.

Place, publisher, year, edition, pages
Wiley, 2022
National Category
Chemical Sciences Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-324128 (URN)10.1002/macp.202200249 (DOI)000896738700001 ()2-s2.0-85144135979 (Scopus ID)
Funder
Swedish Research Council, 2020‐05486
Note

QC 20230228

Available from: 2023-02-21 Created: 2023-02-21 Last updated: 2023-11-30Bibliographically approved
Rostami, J., Benselfelt, T., Maddalena, L., Avci, C., Sellman, F. A., Ciftci, G. C., . . . Wågberg, L. (2022). Shaping 90 wt% NanoMOFs into Robust Multifunctional Aerogels Using Tailored Bio-Based Nanofibrils. Advanced Materials, 34(38), Article ID 2204800.
Open this publication in new window or tab >>Shaping 90 wt% NanoMOFs into Robust Multifunctional Aerogels Using Tailored Bio-Based Nanofibrils
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2022 (English)In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 34, no 38, article id 2204800Article in journal (Refereed) Published
Abstract [en]

Metal–organic frameworks (MOFs) are hybrid porous crystalline networks with tunable chemical and structural properties. However, their excellent potential is limited in practical applications by their hard-to-shape powder form, making it challenging to assemble MOFs into macroscopic composites with mechanical integrity. While a binder matrix enables hybrid materials, such materials have a limited MOF content and thus limited functionality. To overcome this challenge, nanoMOFs are combined with tailored same-charge high-aspect-ratio cellulose nanofibrils (CNFs) to manufacture robust, wet-stable, and multifunctional MOF-based aerogels with 90 wt% nanoMOF loading. The porous aerogel architectures show excellent potential for practical applications such as efficient water purification, CO2 and CH4 gas adsorption and separation, and fire-safe insulation. Moreover, a one-step carbonization process enables these aerogels as effective structural energy-storage electrodes. This work exhibits the unique ability of high-aspect-ratio CNFs to bind large amounts of nanoMOFs in structured materials with outstanding mechanical integrity—a quality that is preserved even after carbonization. The demonstrated process is simple and fully discloses the intrinsic potential of the nanoMOFs, resulting in synergetic properties not found in the components alone, thus paving the way for MOFs in macroscopic multifunctional composites. 

Place, publisher, year, edition, pages
Wiley, 2022
Keywords
aerogels, cellulose nanofibrils, flame retardancy, gas adsorption and separation, metal–organic frameworks, supercapacitors, water purification, Aspect ratio, Carbonization, Crystalline materials, Gas adsorption, Hybrid materials, Nanocellulose, Nanofibers, Supercapacitor, Bio-based, Crystalline networks, Flame-retardancy, Gas adsorption and separations, High aspect ratio, Mechanical integrity, Metalorganic frameworks (MOFs), Nano-fibrils, Binders, Composites, Loading, Materials, Powder, Processes
National Category
Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-326793 (URN)10.1002/adma.202204800 (DOI)000840897400001 ()35906189 (PubMedID)2-s2.0-85135930335 (Scopus ID)
Note

QC 20230515

Available from: 2023-05-15 Created: 2023-05-15 Last updated: 2023-05-15Bibliographically approved
Nordenström, M., Benselfelt, T., Hollertz, R., Wennmalm, S., Larsson, P. A., Mehandzhiyski, A., . . . Wågberg, L. (2022). The structure of cellulose nanofibril networks at low concentrations and their stabilizing action on colloidal particles. Carbohydrate Polymers, 297, 120046, Article ID 120046.
Open this publication in new window or tab >>The structure of cellulose nanofibril networks at low concentrations and their stabilizing action on colloidal particles
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2022 (English)In: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 297, p. 120046-, article id 120046Article in journal (Refereed) Published
Abstract [en]

The structure and dynamics of networks formed by rod-shaped particles can be indirectly investigated by measuring the diffusion of spherical tracer particles. This method was used to characterize cellulose nanofibril (CNF) networks in both dispersed and arrested states, the results of which were compared with coarse-grained Brownian dynamics simulations. At a CNF concentration of 0.2 wt% a transition was observed where, below this concentration tracer diffusion is governed by the increasing macroscopic viscosity of the dispersion. Above 0.2 wt%, the diffusion of small particles (20-40 nm) remains viscosity controlled, while particles (100-500 nm) become trapped in the CNF network. Sedimentation of silica microparticles (1-5 mu m) in CNF dispersions was also determined, showing that sedimentation of larger particles is significantly affected by the presence of CNF. At concentrations of 0.2 wt%, the sedimentation velocity of 5 mu m particles was reduced by 99 % compared to pure water.

Place, publisher, year, edition, pages
Elsevier BV, 2022
Keywords
Cellulose nanofibrils, Colloid stability, Simulations, Diffusion, Sedimentation, Models
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-319717 (URN)10.1016/j.carbpol.2022.120046 (DOI)000860482300005 ()36184183 (PubMedID)2-s2.0-85137161224 (Scopus ID)
Note

QC 20221017

Available from: 2022-10-17 Created: 2022-10-17 Last updated: 2022-12-12Bibliographically approved
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Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0003-4388-8970

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