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Rostami, J., Sellman, F. A., Lillberg, E., Östmans, R., Wågberg, L. & Benselfelt, T. (2025). All-Cellulose Superabsorbent Heterostructures Comprising Fiber Aerogels and Nanofibril Sheets. Chemistry of Materials, 37(9), 3073-3087
Open this publication in new window or tab >>All-Cellulose Superabsorbent Heterostructures Comprising Fiber Aerogels and Nanofibril Sheets
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2025 (English)In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 37, no 9, p. 3073-3087Article in journal (Refereed) Published
Abstract [en]

Superabsorbent polymers (SAPs) are essential components in absorption products for food packaging, agriculture, wound dressings, and hygiene. Modern absorption products are designed to rapidly absorb and transport liquids to SAPs, which drains the porous networks and hold liquids under pressure as hydrogels. However, the carbon footprint of these massively used, fossil-based products is high, leading to an urgent need to develop biobased superabsorbents. Although commercial SAPs have an absorption capacity under load that is challenging to surmount, their powder form complicates processing. Thus, biobased alternatives can compete with other advantages, such as intelligently designed self-supporting structures preferably manufactured in sustainable roll-to-roll processes. As a pioneering step, this study presents all-cellulose superabsorbent heterostructures prepared by combining macroporous fiber-based aerogels with highly swelling cellulose nanofibril (CNF) sheets. The aerogel rapidly absorbs 30 g g-1 of liquid, which is rapidly transferred to the CNF sheets with a maximum capacity of 246 g g-1, holding liquids at pressures of up to 0.9 MPa. The heterostructure is also equipped with a simple, sustainable conductometric water-uptake sensor to follow the liquid uptake and saturation level. Using unmodified raw materials from the forest industry in a scalable process with the potential for roll-to-roll manufacturing makes these all-cellulose heterostructures a competitive alternative to commercial SAPs in a carbon-neutral society.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2025
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-366106 (URN)10.1021/acs.chemmater.4c02926 (DOI)001477018900001 ()2-s2.0-105003737649 (Scopus ID)
Note

QC 20250707

Available from: 2025-07-07 Created: 2025-07-07 Last updated: 2025-07-07Bibliographically approved
Benselfelt, T., Reid, M. S., Edberg, J., Belaineh, D., Fager, C., Subramaniyam, C. M., . . . Wågberg, L. (2025). Membranes and separators from cellulose fibrils of different degrees of refining. Journal of Environmental Chemical Engineering, 13(2), Article ID 115766.
Open this publication in new window or tab >>Membranes and separators from cellulose fibrils of different degrees of refining
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2025 (English)In: Journal of Environmental Chemical Engineering, E-ISSN 2213-3437, Vol. 13, no 2, article id 115766Article in journal (Refereed) Published
Abstract [en]

Membranes and separators are crucial components in many processes and devices. The state-of-the-art fossil-based membranes have a high carbon footprint, and polyfluorinated membranes are increasingly phased out. These limitations lead to an inevitable transition that calls for carbon-neutral membranes with the same or even better performance that can be produced at scale and low cost. Cellulose membranes have the potential to fulfill these criteria if they can be tuned for different purposes. A way to tailor cellulose membranes by preparing them from cellulose fibrils of different refining degrees is presented. The membranes’ effective pore size and permeability to PEG, Fluorescein, and different ions were characterized. The membranes were efficiently used as separators in aqueous-based Zn-ion batteries and PEDOT supercapacitors. This work demonstrates a route toward high-performing and versatile cellulose membranes that can be produced at scale in a more sustainable membrane industry.

Place, publisher, year, edition, pages
Elsevier BV, 2025
Keywords
Batteries, Cellulose, Fibrils, Membranes, Supercapacitors
National Category
Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-360575 (URN)10.1016/j.jece.2025.115766 (DOI)001428726400001 ()2-s2.0-85217783398 (Scopus ID)
Note

QC 20250311

Available from: 2025-02-26 Created: 2025-02-26 Last updated: 2025-03-11Bibliographically approved
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)001224676200001 ()2-s2.0-85189942008 (Scopus ID)
Note

QC 20240424

Available from: 2024-04-18 Created: 2024-04-18 Last updated: 2024-06-03Bibliographically 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
Benselfelt, T., Shakya, J., Rothemund, P., Lindström, S. B., Piper, A., Winkler, T. E., . . . Hamedi, M. (2023). Electrochemically Controlled Hydrogels with Electrotunable Permeability and Uniaxial Actuation. Advanced Materials, 35(45), Article ID 2303255.
Open this publication in new window or tab >>Electrochemically Controlled Hydrogels with Electrotunable Permeability and Uniaxial Actuation
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2023 (English)In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 35, no 45, article id 2303255Article in journal (Refereed) Published
Abstract [en]

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.

Place, publisher, year, edition, pages
Wiley, 2023
Keywords
electrochemical actuation, electronic actuators, hydrogels, nanowires, osmotic pressure, tunable membranes
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-348212 (URN)10.1002/adma.202303255 (DOI)001057441300001 ()2-s2.0-85167722724 (Scopus ID)
Note

QC 20240624

Available from: 2024-06-24 Created: 2024-06-24 Last updated: 2024-06-24Bibliographically 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
Li, L., Tian, W., VahidMohammadi, A., Rostami, J., Chen, B., Matthews, K., . . . Hamedi, M. (2023). Ultrastrong Ionotronic Films Showing Electrochemical Osmotic Actuation. Advanced Materials, 35(45), Article ID 2301163.
Open this publication in new window or tab >>Ultrastrong Ionotronic Films Showing Electrochemical Osmotic Actuation
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2023 (English)In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 35, no 45, article id 2301163Article in journal (Refereed) Published
Abstract [en]

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.

Place, publisher, year, edition, pages
Wiley, 2023
Keywords
cellulose nanofibrils, hydrogel actuators, ionotronic conductivity, MXenes, nanocomposite films
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-348452 (URN)10.1002/adma.202301163 (DOI)001047337200001 ()2-s2.0-85167665653 (Scopus ID)
Note

QC 20240624

Available from: 2024-06-24 Created: 2024-06-24 Last updated: 2024-06-24Bibliographically approved
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Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0003-4388-8970

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