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Jerlhagen, Å., Gordeyeva, K., Cattaruzza, M., Brandt, L., Sochor, B., Koyiloth Vayalil, S., . . . Malmström, E. (2025). Decoding in-plane orientation in cellulose nanopapers hybridized with tailored polymeric nanoparticles. Nanoscale, 17(14), 8712-8723
Open this publication in new window or tab >>Decoding in-plane orientation in cellulose nanopapers hybridized with tailored polymeric nanoparticles
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2025 (English)In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 17, no 14, p. 8712-8723Article in journal (Refereed) Epub ahead of print
Abstract [en]

Biobased cellulose nanofibrils (CNFs) constitute important building blocks for biomimetic, nanostructured materials, and considerable potential exists in their hybridization with tailorable polymeric nanoparticles. CNFs naturally assemble into oriented, fibrillar structures in their cross-section. This work shows that polymeric nanoparticle additives have the potential to increase or decrease orientation of these cellulose structures, which allows the control of bulk mechanical properties. Small amounts of these additives (<1 wt%) are shown to promote the alignment of CNFs, and the particle size is found to determine a tailorable maximum feature size which can be modified. Herein, X-ray scattering allows for the quantification of orientation at different length scales. This newly developed method of measuring cross-sectional orientation allows for understanding the influence of nanoparticle characteristics on the CNF network structure at different length scales in hybrid cellulose-nanoparticle materials, where previously quantitative description has been lacking. It thus constitutes an important foundation for further development and understanding of nanocellulose materials on the level of their nanoscale building blocks and their interactions, which in turn are decisive for their macroscopic properties.

Place, publisher, year, edition, pages
Royal Society of Chemistry (RSC), 2025
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-361628 (URN)10.1039/d4nr04381b (DOI)001444772800001 ()40070204 (PubMedID)2-s2.0-105002162860 (Scopus ID)
Note

QC 20250324

Available from: 2025-03-24 Created: 2025-03-24 Last updated: 2025-05-07Bibliographically 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
Sjölund, J., Westman, G., Wågberg, L. & Larsson, P. A. (2025). On the determination of charge and nitrogen content in cellulose fibres modified to contain quaternary amine functionality. Carbohydrate Polymers, 347, Article ID 122734.
Open this publication in new window or tab >>On the determination of charge and nitrogen content in cellulose fibres modified to contain quaternary amine functionality
2025 (English)In: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 347, article id 122734Article in journal (Refereed) Published
Abstract [en]

Research interest in quaternization of cellulose fibres has increased considerably over the past decades. However, there is little or no consensus regarding how to characterize the material in terms of degree of substitution (DS), and the literature suggests a range of different methods focusing on charge determination as well as nitrogen content quantification. This work aims to fill the knowledge gap regarding how the different methods perform in relation to each other, and for what cellulosic systems each method has advantages, disadvantages and even potential pitfalls. FT-IR and NMR measurements are used to establish successful modification and determine the relative number of substituent groups. Another six methods are compared for the determination of the DS of cellulosic fibres and nanofibrils. The methods include Kjeldahl measurements, nitrogen determination by chemiluminescence, determination of molecular nitrogen by the Dumas method, colloidal titration, conductometric titration and polyelectrolyte adsorption. It can be concluded that most techniques investigated are reliable within certain ranges of DS and/or when using appropriate post-treatment of the quaternized material and suitable sample preparation techniques. The results from the present work hence provide recommendations to make an educated choice of method, and experimental protocol, based on the technique at hand.

Place, publisher, year, edition, pages
Elsevier BV, 2025
Keywords
Cellulose Fibres, Charge determination, Degree of substitution, Nitrogen quantification, Quaternization
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-353929 (URN)10.1016/j.carbpol.2024.122734 (DOI)001316839200001 ()39486964 (PubMedID)2-s2.0-85203849829 (Scopus ID)
Note

QC 20241008

Available from: 2024-09-25 Created: 2024-09-25 Last updated: 2025-05-27Bibliographically approved
Mao, A., Gebhard, A. C., Ezazi, N. Z., Salhotra, A., Riazanova, A., Shanker, R., . . . Svagan, A. J. (2025). Plant cell–inspired colon-targeted cargo delivery systems with dual-triggered release mechanisms. Science Advances, 11(20), Article ID eadt2653.
Open this publication in new window or tab >>Plant cell–inspired colon-targeted cargo delivery systems with dual-triggered release mechanisms
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2025 (English)In: Science Advances, E-ISSN 2375-2548, Vol. 11, no 20, article id eadt2653Article in journal (Refereed) Published
Abstract [en]

Plant cells represent smart cargo carriers with great socioeconomic potential in oral drug delivery applications. The two exterior barriers, featuring a rigid cell wall and a dense plasma membrane, are unique with complementary structural, mechanical, and chemical properties. Current strategies for producing therapeutic drugs within plant cells for oral delivery are efficient, but largely limited to recombinant pharmaceutical proteins, and involve complex genetic modification of plants. To address this, we engineer plant cell–inspired delivery systems with cellulose nanofiber–based shells and lipid layers through a bottom-up assembly strategy, which offers greater flexibility to encapsulate nonprotein compounds and nanoparticles. Notably, the layered shell structure resists degradation in acidic environments, and two barriers respond differently to external stimuli in simulated gastrointestinal medium, resulting in size-dependent dual-triggered release mechanisms. The cytocompatibility was shown by incubation with Caco-2 cells. Our results open avenues for developing next generation of bioinspired oral delivery systems for multisite-specific gastrointestinal release in a low-cost and sustainable manner.

Place, publisher, year, edition, pages
American Association for the Advancement of Science (AAAS), 2025
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-364021 (URN)10.1126/sciadv.adt2653 (DOI)001487911700006 ()40367175 (PubMedID)2-s2.0-105005475987 (Scopus ID)
Note

QC 20250603

Available from: 2025-06-02 Created: 2025-06-02 Last updated: 2025-06-03Bibliographically approved
Cortes Ruiz, M. F., Martin, J., Marcos Celada, L., Olsén, P. & Wågberg, L. (2025). Strategic functionalization of wood fibers for the circular design of fiber-reinforced hydrogel composites. Cell Reports Physical Science, 6(3), Article ID 102455.
Open this publication in new window or tab >>Strategic functionalization of wood fibers for the circular design of fiber-reinforced hydrogel composites
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2025 (English)In: Cell Reports Physical Science, E-ISSN 2666-3864, Vol. 6, no 3, article id 102455Article in journal (Refereed) Published
Abstract [en]

Cellulosic nanomaterials are ideal reinforcers in hydrogel composites, but the current techniques that ensure defined nano-dimensions reduce sustainability. A different strategy for the synthesis of hydrogels from pulp fibers using green chemistry could offer a more sustainable solution. This work explores a mild, straightforward chemical modification with maleic anhydride that simultaneously decorates the fibers with carboxylate and alkene groups. Tuning the temperature of the reaction enables control over the surface charge ranging from 150 to 1,000 μmol/g. The fibers are used to construct a rubber-like, water-stable hydrogel composite prepared by in situ telechelic PEG polymerization followed by thermal or UV-induced free radical crosslinking. The initiation strategy, molecular weight of telechelic PEG, and degree of modification of the fibers enable control over the network formation within and around the fibers. The hydrogel composite is designed to be hydrolytically degradable under alkaline conditions, allowing separate recovery of both fibers and polymer precursors.

Place, publisher, year, edition, pages
Elsevier BV, 2025
Keywords
cellulose, circular materials, degradable, hydrogels, in situ polymerization, radical polymerization, surface modification, wood-based fibers
National Category
Polymer Chemistry Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-361783 (URN)10.1016/j.xcrp.2025.102455 (DOI)001452416400001 ()2-s2.0-86000754314 (Scopus ID)
Note

QC 20250428

Available from: 2025-03-27 Created: 2025-03-27 Last updated: 2025-04-28Bibliographically approved
Liu, M., Zhang, L., Rostami, J., Zhang, T., Matthews, K., Chen, S., . . . Gogotsi, Y. (2025). Tough MXene-Cellulose Nanofibril Ionotronic Dual-Network Hydrogel Films for Stable Zinc Anodes. ACS Nano, 19(13), 13399-13413
Open this publication in new window or tab >>Tough MXene-Cellulose Nanofibril Ionotronic Dual-Network Hydrogel Films for Stable Zinc Anodes
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2025 (English)In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 19, no 13, p. 13399-13413Article in journal (Refereed) Published
Abstract [en]

Developing ionotronic interface layers for zinc anodes with superior mechanical integrity is one of the efficient strategies to suppress the growth of zinc dendrites in favor of the cycling stability of aqueous zinc-ion batteries (AZIBs). Herein, we assembled robust 2D MXene-based hydrogel films cross-linked by 1D cellulose nanofibril (CNF) dual networks, acting as interface layers to stabilize Zn anodes. The MXene-CNF hydrogel films integrated multifunctionalities, including a high in-plane toughness of 18.39 MJ m-3, high in-plane/out-of-plane elastic modulus of 0.85 and 3.65 GPa, mixed electronic/ionic (ionotronic) conductivity of 1.53 S cm-1 and 0.52 mS cm-1, and high zincophilicity with a high binding energy (1.33 eV) and low migration energy barrier (0.24 eV) for Zn2+. These integrated multifunctionalities, endowed with coupled multifield effects, including strong stress confinement and uniform ionic/electronic field distributions on Zn anodes, effectively suppressed dendrite growth, as proven by experiments and simulations. An example of the MXene-CNF|Zn showed a reduced nucleation overpotential of 19 mV, an extended cycling life of over 2700 h in Zn||Zn cells, and a high capacity of 323 mAh g-1 in Zn||MnO2 cells, compared with bare Zn. This work offers an approach for exploring mechanically robust 1D/2D ionotronic hydrogel interface layers to stabilize the Zn anodes of AZIBs.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2025
Keywords
cellulose nanofibrils, interface layers, Ionotronic hydrogel, MXene, zinc anodes
National Category
Materials Chemistry Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-362728 (URN)10.1021/acsnano.5c01497 (DOI)001451671200001 ()40130552 (PubMedID)2-s2.0-105002485153 (Scopus ID)
Note

QC 20250425

Available from: 2025-04-23 Created: 2025-04-23 Last updated: 2025-04-25Bibliographically approved
Lander, S., Pang, J., Erlandsson, J., Vagin, M., Jafari, M. J., Korhonen, L., . . . Berggren, M. (2024). Controlling the rate of posolyte degradation in all-quinone aqueous organic redox flow batteries by sulfonated nanocellulose based membranes: The role of crossover and Michael addition. Journal of Energy Storage, 83, Article ID 110338.
Open this publication in new window or tab >>Controlling the rate of posolyte degradation in all-quinone aqueous organic redox flow batteries by sulfonated nanocellulose based membranes: The role of crossover and Michael addition
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2024 (English)In: Journal of Energy Storage, ISSN 2352-152X, E-ISSN 2352-1538, Vol. 83, article id 110338Article in journal (Refereed) Published
Abstract [en]

Aqueous organic redox flow battery (AORFB) is a technological route towards the large-scale sustainable energy storage. However, several factors need to be controlled to maintain the AORFB performance. Prevention of posolyte and negolyte cross-contamination in asymmetric AORFBs, one of the main causes of capacity decay, relies on their membranes' ability to prevent migration of the redox-active species between the two electrolytes. The barrier properties are often traded for a reduction in ionic conductivity which is crucial to enable the device operation. Another factor greatly affecting quinone-based AORFBs is the Michael addition reaction (MAR) on the charged posolyte, quinone, which has been identified as a major reason for all-quinone AORFBs performance deterioration. Herein, we investigate deterioration scenarios of an all-quinone AORFB using both experimental and computational methods. The study includes a series of membranes based on sulfonated cellulose nanofibrils and different membrane modifications. The layer-by-layer (LbL) surface modifications, i.e. the incorporation of inorganic materials and the reduction of the pore size of the sulfonated cellulose membranes, were all viable routes to reduce the passive diffusion permeability of membranes which correlated to an increased cycling stability of the battery. The kinetics of MAR on quinone was detected using NMR and its impact on the performance fading was modeled computationally. The localization of MAR close to the membrane, which can be assigned to the surface reactivity, affects the diffusion of MAR reagent and the deterioration dynamics of the present all-quinone AORFB.

Place, publisher, year, edition, pages
Elsevier BV, 2024
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-343674 (URN)10.1016/j.est.2023.110338 (DOI)2-s2.0-85184521391 (Scopus ID)
Note

QC 20240222

Available from: 2024-02-22 Created: 2024-02-22 Last updated: 2024-02-22Bibliographically approved
Brooke, R., Jain, K., Isacsson, P., Fall, A., Engquist, I., Beni, V., . . . Edberg, J. (2024). Digital Cellulose: Recent Advances in Electroactive Paper. Annual review of materials research (Print), 54, 1-25
Open this publication in new window or tab >>Digital Cellulose: Recent Advances in Electroactive Paper
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2024 (English)In: Annual review of materials research (Print), ISSN 1531-7331, E-ISSN 1545-4118, Vol. 54, p. 1-25Article, review/survey (Refereed) Published
Abstract [en]

With the increasing global demand for net-zero carbon emissions, actions to address climate change have gained momentum among policymakers and the public. The urgent need for a sustainable economy is underscored by the mounting waste crisis in landfills and oceans. However, the proliferation of distributed electronic devices poses a significant challenge due to the resulting electronic waste. To combat this issue, the development of sustainable and environmentally friendly materials for these devices is imperative. Cellulose, an abundant and CO2-neutral substance with a long history of diverse applications, holds great potential. By integrating electrically interactive components with cellulosic materials, innovative biobased composites have been created, enabling the fabrication of bulk electroactive paper and the establishment of new, potentially more sustainable manufacturing processes for electronic devices. This review explores recent advances in bulk electroactive paper, including the fundamental interactions between its constituents, manufacturing techniques, and large-scale applications in the field of electronics. Furthermore, it addresses the importance and challenges of scaling up production of electroactive paper, highlighting the need for further research and development.

Place, publisher, year, edition, pages
Annual Reviews, 2024
Keywords
cellulose, nanocellulose, cellulose nanofibrils, composites, electroactive paper, conductive polymers
National Category
Materials Engineering
Identifiers
urn:nbn:se:kth:diva-354339 (URN)10.1146/annurev-matsci-080921-084430 (DOI)001285374800001 ()2-s2.0-85206295715 (Scopus ID)
Note

QC 20241003

Available from: 2024-10-03 Created: 2024-10-03 Last updated: 2025-05-27Bibliographically approved
Elf, P., Larsson, P. A., Larsson, A., Wågberg, L., Hedenqvist, M. S. & Nilsson, F. (2024). Effects of Ring Opening and Chemical Modification on the Properties of Dry and Moist Cellulose─Predictions with Molecular Dynamics Simulations. Biomacromolecules, 25(12), 7581-7593
Open this publication in new window or tab >>Effects of Ring Opening and Chemical Modification on the Properties of Dry and Moist Cellulose─Predictions with Molecular Dynamics Simulations
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2024 (English)In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 25, no 12, p. 7581-7593Article in journal (Refereed) Published
Abstract [en]

Thermoplastic properties in cellulosic materials can be achieved by opening the glucose rings in cellulose and introducing new functional groups. Using molecular dynamics, we simulated amorphous cellulose and eight modified versions under dry and moist conditions. Modifications included ring openings and functionalization with hydroxy, aldehyde, hydroxylamine, and carboxyl groups. These modifications were analyzed for density, glass transition temperature, thermal expansivity, hydrogen bond features, changes in energy term contributions during deformation, diffusivity, free volume, and tensile properties. All ring-opened systems exhibited higher molecular mobility, which, consequently, improved thermoplasticity (processability) compared to that of the unmodified amorphous cellulose. Dialcohol cellulose and hydroxylamine-functionalized cellulose were identified as particularly interesting due to their combination of high molecular mobility at processing temperatures (425 K) and high stiffness and strength at room temperature (300 K). Water and smaller side groups improved processability, indicating that both steric effects and electrostatics have a key role in determining the processability of polymers.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2024
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-362972 (URN)10.1021/acs.biomac.4c00735 (DOI)001362815500001 ()39586018 (PubMedID)2-s2.0-85210410701 (Scopus ID)
Funder
Vinnova, 201900047
Note

QC 20250502

Available from: 2025-04-30 Created: 2025-04-30 Last updated: 2025-05-02Bibliographically approved
Asta, N., Kaplan, M., Kulachenko, A., Östlund, S. & Wågberg, L. (2024). Influence of density and chemical additives on paper mechanical properties. Cellulose, 31(9), 5809-5822
Open this publication in new window or tab >>Influence of density and chemical additives on paper mechanical properties
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2024 (English)In: Cellulose, ISSN 0969-0239, E-ISSN 1572-882X, Vol. 31, no 9, p. 5809-5822Article in journal (Refereed) Published
Abstract [en]

In this work we have investigated the effect of surface modification of fibres on the overall mechanical properties of high-density papers. Paper sheets were prepared by a combination of heat-pressing and polyelectrolyte Layer-by-Layer (LbL) modification of different softwood fibres. LbLs of Polyallylamine Hydrochloride (PAH) and Hyaluronic Acid (HA) were adsorbed onto unbleached kraft fibres and bleached Chemo-ThermoMechanical Pulp (CTMP) to improve the strength of the fibre–fibre joints in papers made from these fibres. Additionally, different sheet-making procedures were used to prepare a range of network densities with different degrees of fibre–fibre interaction in the system. The results demonstrate that interfacial adhesion within fibre–fibre joints plays a pivotal role in the network's performance, even at higher paper densities. Hygroexpansion measurements and fracture zone imaging with Scanning Electron Microscopy (SEM) further support the claim that stronger interactions between the fibres allow for a better utilisation of the inherent fibre properties. Surface treatments and network densification significantly improved the paper sheets' mechanical properties. Specifically, LbL-treatments alone increased specific stiffness up to 60% and specific strength by over 100%. This improvement is linked to the build-up of residual stresses during drying. Due to a high interaction between the fibres during water removal the fibres become constrained, leading to increased stretching of fibre segments. Strengthened fibre joints intensify this constraint, further increasing the stretch and, consequently, the paper's strength.

Keywords
high-density networks; layer-by-layer self assembly; surface modification; hygroexpansion; joint strength; paper mechanical properties
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-359150 (URN)10.1007/s10570-024-05917-6 (DOI)001215584700003 ()2-s2.0-85192364564 (Scopus ID)
Funder
Stora EnsoKnut and Alice Wallenberg Foundation, Dnr KAW 2018.0451
Note

Not duplicate with DiVA 1849242

QC 20250127

Available from: 2025-01-27 Created: 2025-01-27 Last updated: 2025-02-18Bibliographically approved
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ORCID iD: ORCID iD iconorcid.org/0000-0001-8622-0386

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