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Ion Transport in Cross-linked Nanocellulose Membranes
Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
2023 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Ion-selective membranes, which allow ions with a certain charge and/or size to pass through while blocking other ions, have attracted much attention due to their diverse applications and outstanding roles in overcoming problems related to energy. In addition to the performance, the financial cost and renewability of materials are equally significant in the development of these membranes. Commonly, ion-selective membranes are prepared from traditional synthetic polymers that have put a heavy burden on the environment. Therefore, exploring low-cost, environment-friendly materials as the substitution of traditional polymers for ion-selective membranes will be beneficial from a sustainable perspective.

Nanocellulose is a promising candidate for the next generation of ionic membranes due to its unique chemical structure and suitable physical dimensions. Furthermore, it can be produced from cellulose, which is the most abundant biopolymer on earth. Nanocellulose has many hydroxyl groups that provide many possibilities to introduce ion-functionalized groups on the cellulose chain through chemical treatment and modification. In addition, the physical entanglement of cellulose nanofibrils can generate a nanoscale porous structure that improves the ion permselectivity of membranes and provides a strong network that enhances the toughness of membranes. Among the disadvantages of nanocellulose-based products is poor wet stability due to the swelling induced by their hydrophilicity. This problem can be effectively solved using covalent cross-linking.

This thesis aims to develop nanocellulose-based ionic membranes with excellent ionic transport properties as well as good wet stability and to explore their potential applications. First, the nanocellulose membranes cross-linked by 1,2,3,4-butanetetracarboxylic acid (BTCA) were developed. The relationship between the amount of cross-linker and the membranes’ pore size, charge density, and ionic transport properties was demonstrated. Based on the above fundamental understanding of the membranes’ performance, especially ion conductivity, and selectivity, their performance was then investigated in two potential applications, including osmotic power generators and redox flow batteries. Finally, the original cross-linked membrane, which is negatively charged, was combined with a corresponding membrane with positive surface charges to obtain bipolar membranes, which can be used for rectification. The properties of these bipolar membranes were investigated, with the conclusion that they can be used as an ionic diode under certain conditions.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2023. , p. 68
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 2299
Keywords [en]
Membranes, Nanocellulose, Cross-linking, Ion transport, Energy harvesting and storage devices
National Category
Polymer Chemistry
Identifiers
URN: urn:nbn:se:liu:diva-193163DOI: 10.3384/9789180750837ISBN: 9789180750820 (print)ISBN: 9789180750837 (electronic)OAI: oai:DiVA.org:liu-193163DiVA, id: diva2:1751429
Public defence
2023-05-23, K1, Kåkenhus, Campus Norrköping, Norrköping, 09:15 (English)
Opponent
Supervisors
Available from: 2023-04-18 Created: 2023-04-18 Last updated: 2023-04-18Bibliographically approved
List of papers
1. The effect of crosslinking on ion transport in nanocellulose-based membranes
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 Science Ltd, 2022
Keywords
Nanocellulose; Membrane; Ion conductivity; Ion selectivity; Crosslinking
National Category
Materials Chemistry
Identifiers
urn:nbn:se:liu:diva-183780 (URN)10.1016/j.carbpol.2021.118938 (DOI)000760950500005 ()34973756 (PubMedID)
Note

Funding Agencies|Digital Cellulose Centre; Wallenberg Wood Science Center (Knut and Alice Wallenberg Foundation); Karl-Erik Onnesjo Foundation; Treesearch, a collaboration platform for Swedish forest industrial research

Available from: 2022-03-25 Created: 2022-03-25 Last updated: 2023-04-18
2. Cross-Linked Nanocellulose Membranes for Nanofluidic Osmotic Energy Harvesting
Open this publication in new window or tab >>Cross-Linked Nanocellulose Membranes for Nanofluidic Osmotic Energy Harvesting
2022 (English)In: ACS Applied Energy Materials, E-ISSN 2574-0962, Vol. 5, no 12, p. 15740-15748Article in journal (Refereed) Published
Abstract [en]

Osmotic energy generated from the salinity gradient is a kind of clean and renewable energy source, where the ion-exchange membranes play a critical role in its operation. The nanofluidic technique is emerging to overcome the limitations of high resistance and low mass transport of traditional ion-exchange membranes and thus improve osmotic power conversion. However, the currently reported nanofluidic materials suffer from high cost and complicated fabrication processes, which limits their practical application. Here, we report low-cost nanocellulose membranes that can be facilely prepared by a chemical cross-linking approach. The obtained membranes exhibit excellent ion transport characteristics as high-performance nanofluidic osmotic power generators. The control of cross-linker dosage enables the simultaneous tunability of the surface charge density and size of nanofluidic channels created between the interwoven cellulose nanofibrils. The maximum osmotic power generated by the membrane is reached when the cross-linker weight content is 20 wt %. Furthermore, the cross-linked nanocellulose membranes exhibit long-term working stability in osmotic energy harvesting under a wide range of pH values (3.2-9.7). This nanocellulose membrane derived from green and sustainable natural materials demonstrates a promising potential for renewable osmotic energy harvesting.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2022
Keywords
nanocellulose; membrane; osmotic energy; nanofluidic; ion selectivity
National Category
Energy Systems
Identifiers
urn:nbn:se:liu:diva-190788 (URN)10.1021/acsaem.2c03308 (DOI)000899478400001 ()
Note

Funding Agencies|Digital Cellulose Center (Swedish Innovation Agency VINNOVA); Wallenberg Wood Science Center (Knut and Alice Wallenberg Foundation); Karl-Erik Onnesjo Foundation

Available from: 2023-01-02 Created: 2023-01-02 Last updated: 2024-02-13Bibliographically approved

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