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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)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
Yang, H., Edberg, J., Say, M. G., Erlandsson, J., Gueskine, V., Wågberg, L., . . . Engquist, I. (2024). Study on the Rectification of Ionic Diode Based on Cross-Linked Nanocellulose Bipolar Membranes. Biomacromolecules, 25(3), 1933-1941
Open this publication in new window or tab >>Study on the Rectification of Ionic Diode Based on Cross-Linked Nanocellulose Bipolar Membranes
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2024 (English)In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 25, no 3, p. 1933-1941Article in journal (Refereed) Published
Abstract [en]

Nanocellulose-based membranes have attracted intense attention in bioelectronic devices due to their low cost, flexibility, biocompatibility, degradability, and sustainability. Herein, we demonstrate a flexible ionic diode using a cross-linked bipolar membrane fabricated from positively and negatively charged cellulose nanofibrils (CNFs). The rectified current originates from the asymmetric charge distribution, which can selectively determine the direction of ion transport inside the bipolar membrane. The mechanism of rectification was demonstrated by electrochemical impedance spectroscopy with voltage biases. The rectifying behavior of this kind of ionic diode was studied by using linear sweep voltammetry to obtain current-voltage characteristics and the time dependence of the current. In addition, the performance of cross-linked CNF diodes was investigated while changing parameters such as the thickness of the bipolar membranes, the scanning voltage range, and the scanning rate. A good long-term stability due to the high density cross-linking of the diode was shown in both current-voltage characteristics and the time dependence of current.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2024
National Category
Electrical Engineering, Electronic Engineering, Information Engineering
Identifiers
urn:nbn:se:kth:diva-344593 (URN)10.1021/acs.biomac.3c01353 (DOI)001182503300001 ()38324476 (PubMedID)2-s2.0-85187301389 (Scopus ID)
Note

QC 20240326

Available from: 2024-03-20 Created: 2024-03-20 Last updated: 2024-03-26Bibliographically approved
Görür, Y. C., Francon, H., Sethi, J., Maddalena, L., Montanari, C., Reid, M. S., . . . Wågberg, L. (2022). Rapidly Prepared Nanocellulose Hybrids as Gas Barrier, Flame Retardant, and Energy Storage Materials. ACS Applied Nano Materials, 5(7), 9188-9200
Open this publication in new window or tab >>Rapidly Prepared Nanocellulose Hybrids as Gas Barrier, Flame Retardant, and Energy Storage Materials
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2022 (English)In: ACS Applied Nano Materials, E-ISSN 2574-0970, Vol. 5, no 7, p. 9188-9200Article in journal (Refereed) Published
Abstract [en]

Cellulose nanofibril (CNF) hybrid materials show great promise as sustainable alternatives to oil-based plastics owing to their abundance and renewability. Nonetheless, despite the enormous success achieved in preparing CNF hybrids at the laboratory scale, feasible implementation of these materials remains a major challenge due to the time-consuming and energy-intensive extraction and processing of CNFs. Here, we describe a scalable materials processing platform for rapid preparation (<10 min) of homogeneously distributed functional CNF-gibbsite and CNF-graphite hybrids through a pH-responsive self-assembly mechanism, followed by their application in gas barrier, flame retardancy, and energy storage materials. Incorporation of 5 wt % gibbsite results in strong, transparent, and oxygen barrier CNF-gibbsite hybrid films in 9 min. Increasing the gibbsite content to 20 wt % affords them self-extinguishing properties, while further lowering their dewatering time to 5 min. The strategy described herein also allows for the preparation of freestanding CNF-graphite hybrids (90 wt % graphite) that match the energy storage performance (330 mA h/g at low cycling rates) and processing speed (3 min dewatering) of commercial graphite anodes. Furthermore, these ecofriendly electrodes can be fully recycled, reformed, and reused while maintaining their initial performance. Overall, this versatile concept combines a green outlook with high processing speed and material performance, paving the way toward scalable processing of advanced ecofriendly hybrid materials. 

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2022
Keywords
CNF, functional hybrids, gibbsite, green materials, nanocomposites, self-assembly, Dewatering, Energy storage, Environmental protection, Exfoliation (materials science), Film preparation, Graphene oxide, Graphite, Nanocellulose, Self assembly, Storage (materials), Supercapacitor, Cellulose nanofibrils, Eco-friendly, Energy storage materials, Functional hybrid, Gas barrier, Gibbsites, Hybrids material, Nano-cellulose, Processing speed, Hybrid materials, Energy, Hybrids, Materials, Performance, Processing, Storage, Water Removal
National Category
Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-326185 (URN)10.1021/acsanm.2c01530 (DOI)000820597300001 ()2-s2.0-85135084223 (Scopus ID)
Note

QC 20230502

Available from: 2023-05-02 Created: 2023-05-02 Last updated: 2023-05-02Bibliographically approved
Lander, S., Vagin, M., Gueskine, V., Erlandsson, J., Boissard, Y., Korhonen, L., . . . Crispin, X. (2022). Sulfonated Cellulose Membranes Improve the Stability of Aqueous Organic Redox Flow Batteries. Advanced Energy and Sustainability Research, 3(9), Article ID 2200016.
Open this publication in new window or tab >>Sulfonated Cellulose Membranes Improve the Stability of Aqueous Organic Redox Flow Batteries
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2022 (English)In: Advanced Energy and Sustainability Research, E-ISSN 2699-9412, Vol. 3, no 9, article id 2200016Article in journal (Refereed) Published
Abstract [en]

The drawbacks of current state-of-the-art selective membranes, such as poor barrier properties, high cost, and poor recyclability, limit the large-scale deployment of electrochemical energy devices such as redox flow batteries (RFBs) and fuel cells. In recent years, cellulosic nanomaterials have been proposed as a low-cost and green raw material for such membranes, but their performance in RFBs and fuel cells is typically poorer than that of the sulfonated fluoropolymer ionomer membranes such as Nafion. Herein, sulfonated cellulose nanofibrils densely cross-linked to form a compact sulfonated cellulose membrane with limited swelling and good stability in water are used. The membranes possess low porosity and excellent ionic transport properties. A model aqueous organic redox flow battery (AORFB) with alizarin red S as negolyte and tiron as posolyte is assembled with the sulfonated cellulose membrane. The performance of the nanocellulose-based battery is superior in terms of cyclability in comparison to that displayed by the battery assembled with commercially available Nafion 115 due to the mitigation of crossover of the redox-active components. This finding paves the way to new green organic materials for fully sustainable AORFB solutions.

Place, publisher, year, edition, pages
Wiley, 2022
Keywords
aqueous organic redox flow batteries, crossover, ion-selective membranes, nanocellulose
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-335676 (URN)10.1002/aesr.202200016 (DOI)000823291000001 ()2-s2.0-85149355399 (Scopus ID)
Note

QC 20230908

Available from: 2023-09-08 Created: 2023-09-08 Last updated: 2023-09-08Bibliographically approved
Lander, S., Erlandsson, J., Vagin, M., Gueskine, V., Korhonen, L., Berggren, M., . . . Crispin, X. (2022). Sulfonated Cellulose Membranes: Physicochemical Properties and Ionic Transport versus Degree of Sulfonation. Advanced Sustainable Systems, 6(11), Article ID 2200275.
Open this publication in new window or tab >>Sulfonated Cellulose Membranes: Physicochemical Properties and Ionic Transport versus Degree of Sulfonation
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2022 (English)In: Advanced Sustainable Systems, E-ISSN 2366-7486, Vol. 6, no 11, article id 2200275Article in journal (Refereed) Published
Abstract [en]

The next generation of green ion selective membranes is foreseen to be based on cellulosic nanomaterials with controllable properties. The introduction of ionic groups into the cellulose structure via chemical modification is one strategy to obtain desired functionalities. In this work, bleached softwood fibers are oxidatively sulfonated and thereafter homogenized to liberate the cellulose nanofibrils (CNFs) from the fiber walls. The liberated CNFs are subsequently used to prepare and characterize novel cellulose membranes. It is found that the degree of sulfonation collectively affects several important properties of the membranes via the density of fixed charged groups on the surfaces of the CNFs, in particular the membrane morphology, water uptake and swelling, and correspondingly the ionic transport. Both ionic conductivity and cation transport increase with the increased level of sulfonation of the starting material. Thus, it is shown that the chemical modification of the CNFs can be used as a tool for precise and rational design of green ion selective membranes that can replace expensive conventional fluorinated ionomer membranes.

Place, publisher, year, edition, pages
Wiley, 2022
Keywords
crosslinked sulfonated nanocelluloses, ionic transport, pore sizes, selective membranes, water uptake
National Category
Polymer Chemistry Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-329048 (URN)10.1002/adsu.202200275 (DOI)000846651200001 ()2-s2.0-85136883902 (Scopus ID)
Note

QC 20230614

Available from: 2023-06-15 Created: 2023-06-15 Last updated: 2023-06-15Bibliographically approved
Yang, H., Edberg, J., Gueskine, V., Vagin, M., Say, M. G., Erlandsson, J., . . . Berggren, M. (2022). The effect of crosslinking on ion transport in nanocellulose-based membranes. Carbohydrate Polymers, 278, Article ID 118938.
Open this publication in new window or tab >>The effect of crosslinking on ion transport in nanocellulose-based membranes
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2022 (English)In: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 278, article id 118938Article in journal (Refereed) Published
Abstract [en]

Ion selective membranes are at the heart of energy conversion and harvesting, water treatment, and biotechnologies. The currently available membranes are mostly based on expensive and non-biodegradable polymers. Here, we report a cation-selective and low-cost membrane prepared from renewable nanocellulose and 1,2,3,4-butanetetracarboxylic acid which simultaneously serves as crosslinker and source of anionic surface groups. Charge density and structure of the membranes are studied. By using different degrees of crosslinking, simultaneous control over both the nanochannel structure and surface charge concentration is achieved, which in turn determines the resulting ion transport properties. Increasing negative charge concentration via higher crosslinker content, the obtained ion conductivity reaches up to 8 mS/cm (0.1 M KCl). Optimal ion selectivity, also influenced by the solution pH, is achieved at 20 wt% crosslinker addition (with ion conductivity of 1.6 mS/cm). As regular similar to 1.4 nm nanochannels were formed at this composition, nanofluidic contribution to ion transport is likely.

Place, publisher, year, edition, pages
Elsevier BV, 2022
Keywords
Nanocellulose, Membrane, Ion conductivity, Ion selectivity, Crosslinking
National Category
Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-310054 (URN)10.1016/j.carbpol.2021.118938 (DOI)000760950500005 ()34973756 (PubMedID)2-s2.0-85120652221 (Scopus ID)
Note

QC 20220322

Available from: 2022-03-22 Created: 2022-03-22 Last updated: 2022-06-25Bibliographically approved
Wang, Z., VahidMohammadi, A., Ouyang, L., Erlandsson, J., Tai, C.-W., Wågberg, L. & Hamedi, M. (2021). Layer-by-Layer Self-Assembled Nanostructured Electrodes for Lithium-Ion Batteries. Small, 17(6), Article ID 2006434.
Open this publication in new window or tab >>Layer-by-Layer Self-Assembled Nanostructured Electrodes for Lithium-Ion Batteries
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2021 (English)In: Small, ISSN 1613-6810, E-ISSN 1613-6829, Vol. 17, no 6, article id 2006434Article in journal (Refereed) Published
Abstract [en]

Gaining control over the nanoscale assembly of different electrode components in energy storage systems can open the door for design and fabrication of new electrode and device architectures that are not currently feasible. This work presents aqueous layer-by-layer (LbL) self-assembly as a route towards design and fabrication of advanced lithium-ion batteries (LIBs) with unprecedented control over the structure of the electrode at the nanoscale, and with possibilities for various new designs of batteries beyond the conventional planar systems. LbL self-assembly is a greener fabrication route utilizing aqueous dispersions that allow various Li+ intercalating materials assembled in complex 3D porous substrates. The spatial precision of positioning of the electrode components, including ion intercalating phase and electron-conducting phase, is down to nanometer resolution. This capable approach makes a lithium titanate anode delivering a specific capacity of 167 mAh g−1 at 0.1C and having comparable performances to conventional slurry-cast electrodes at current densities up to 100C. It also enables high flexibility in the design and fabrication of the electrodes where various advanced multilayered nanostructures can be tailored for optimal electrode performance by choosing cationic polyelectrolytes with different molecular sizes. A full-cell LIB with excellent mechanical resilience is built on porous insulating foams. 

Place, publisher, year, edition, pages
Wiley-VCH Verlag, 2021
Keywords
3D electrodes, compressible batteries, energy storage, nanomaterials, self-assembly, Electrodes, Fabrication, Ions, Lithium compounds, Nanotechnology, Polyelectrolytes, Substrates, Advanced lithium-ion batteries, Cationic polyelectrolyte, Conventional slurries, Device architectures, Energy storage systems, Multilayered nanostructures, Nano-structured electrodes, Nanometer resolutions, Lithium-ion batteries
National Category
Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-292535 (URN)10.1002/smll.202006434 (DOI)000603151700001 ()33373094 (PubMedID)2-s2.0-85098124739 (Scopus ID)
Note

QC 20210409

Available from: 2021-04-09 Created: 2021-04-09 Last updated: 2024-01-09Bibliographically approved
Nordenström, M., Kaldéus, T., Erlandsson, J., Pettersson, T., Malmström, E. & Wågberg, L. (2021). Redispersion Strategies for Dried Cellulose Nanofibrils. ACS Sustainable Chemistry and Engineering, 9(33), 11003-11010
Open this publication in new window or tab >>Redispersion Strategies for Dried Cellulose Nanofibrils
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2021 (English)In: ACS Sustainable Chemistry and Engineering, E-ISSN 2168-0485, Vol. 9, no 33, p. 11003-11010Article in journal (Refereed) Published
Abstract [en]

The potential for large-scale applications of cellulose nanofibrils (CNFs) is limited by the high water content of the starting material, which leads to high transportation costs and undesirable environmental impact. However, drying of CNFs results in loss of their nanoscopic dimensions leading to deterioration of their unique inherent mechanical properties. Herein, thorough redispersion studies of both fundamental and applied nature have been conducted in order to evaluate the effect of charge, redispersing agent, and drying method. Freeze-dried CNF dispersions were successfully redispersed by either increasing the charge density or adding redispersing agents. The greatest effect on redispersibility was achieved with fractionated LignoBoost lignin as redispersing agent, and this is attributed to steric repulsion during water removal and reduced CNF adhesion. Furthermore, the results unexpectedly show that redispersion is easier when the CNFs are dried in the form of nanopapers. By using this approach, excellent redispersibility was achieved even without a redispersing agent. Nanopapers formed from the redispersed CNFs was found to have essentially the same mechanical properties as those made from never-dried CNFs. Hence, this work suggests solutions for making CNFs viable for large-scale application while maintaining their nanoscale dimensions and their ability to create nanopapers with excellent mechanical properties.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2021
Keywords
Cellulose nanofibrils, Redispersibility, Colloidal stability, Redispersing agents, Nanopapers, Mechanical properties
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-301826 (URN)10.1021/acssuschemeng.1c02122 (DOI)000689137600004 ()2-s2.0-85113837473 (Scopus ID)
Note

QC 20210915

Available from: 2021-09-15 Created: 2021-09-15 Last updated: 2022-06-25Bibliographically approved
Wågberg, L. & Erlandsson, J. (2021). The Use of Layer-by-Layer Self-Assembly and Nanocellulose to Prepare Advanced Functional Materials. Advanced Materials, 33(28), Article ID 2001474.
Open this publication in new window or tab >>The Use of Layer-by-Layer Self-Assembly and Nanocellulose to Prepare Advanced Functional Materials
2021 (English)In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 33, no 28, article id 2001474Article, review/survey (Refereed) Published
Abstract [en]

The current knowledge about the formation of layer-by-layer (LbL) self-assemblies using combinations of nanocelluloses (NCs) and polyelectrolytes is reviewed. Herein, the fundamentals behind the LbL formation, with a major focus on NCs, are considered. Following this, a special description of the limiting factors for the formation of LbLs of only NCs, both anionic and cationic, and the combination of NCs and polyelectrolytes/nanoparticles is provided. The ability of the NCs and polyelectrolytes to form dense films with excellent mechanical properties and with tailored optical properties is then reviewed. How low-density, wet stable networks of cellulose nanofibrils can be used as substrates for the preparation of antibacterial, electrically interactive, and fire-retardant materials by forming well-defined LbLs inside these networks is then considered. A short outlook of the possible uses of LbLs containing NCs is given to conclude.

Place, publisher, year, edition, pages
Wiley, 2021
Keywords
cellulose nanocrystals, cellulose nanofibrils, layer-by-layer structures, polyelectrolytes
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-303486 (URN)10.1002/adma.202001474 (DOI)000556252500001 ()32767441 (PubMedID)2-s2.0-85089076696 (Scopus ID)
Note

QC 20211014

Available from: 2021-10-14 Created: 2021-10-14 Last updated: 2022-06-25Bibliographically approved
Han, S., Ruoko, T.-P. -., Gladisch, J., Erlandsson, J., Wågberg, L., Crispin, X. & Fabiano, S. (2020). Cellulose-Conducting Polymer Aerogels for Efficient Solar Steam Generation. Advanced Sustainable Systems, 4(7), 2000004
Open this publication in new window or tab >>Cellulose-Conducting Polymer Aerogels for Efficient Solar Steam Generation
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2020 (English)In: Advanced Sustainable Systems, ISSN 2366-7486, Vol. 4, no 7, p. 2000004-Article in journal (Refereed) Published
Abstract [en]

Seawater desalination and wastewater purification technologies are the main strategies against the global fresh water shortage. Among these technologies, solar-driven evaporation is effective in extracting fresh water by efficiently exploiting solar energy. However, building a sustainable and low-cost solar steam generator with high conversion efficiency is still a challenge. Here, pure organic aerogels comprising a cellulose scaffold decorated with an organic conducting polymer absorbing in the infrared are employed to establish a high performance solar steam generator. The low density of the aerogel ensures minimal material requirements, while simultaneously satisfying efficient water transport. To localize the absorbed solar energy and make the system floatable, a porous floating and thermal-insulating foam is placed between the water and the aerogel. Thanks to the high absorbance of the aerogel and the thermal-localization performance of the foam, the system exhibits a high water evaporation rate of 1.61 kg m−2 h−1 at 1 kW m−2 under 1 sun irradiation, which is higher than most reported solar steam generation devices. 

Place, publisher, year, edition, pages
Wiley-VCH Verlag, 2020
Keywords
cellulose aerogels, freeze-drying, PEDOT:PSS, solar steam generation, water purification
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-274226 (URN)10.1002/adsu.202000004 (DOI)000527086300001 ()2-s2.0-85083643908 (Scopus ID)
Note

QC 20200707

Available from: 2020-07-07 Created: 2020-07-07 Last updated: 2022-06-26Bibliographically approved
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ORCID iD: ORCID iD iconorcid.org/0000-0003-1874-2187

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