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Effects of Different Manufacturing Processes on TEMPO-Oxidized Carboxylated Cellulose Nanofiber Performance as Binder for Flexible Lithium-Ion Batteries
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK). KTH Royal Institute of Technology, Sweden.
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK). KTH Royal Institute of Technology, Sweden.ORCID iD: 0000-0002-0671-435X
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Number of Authors: 62017 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 9, no 43, p. 37712-37720Article in journal (Refereed) Published
Abstract [en]

Carboxylated cellulose nanofibers (CNF) prepared using the TEMPO-route are good binders of electrode components in flexible lithium-ion batteries (LIB). However, the different parameters employed for the defibrillation of CNF such as charge density and degree of homogenization affect its properties when used as binder. This work presents a systematic study of CNF prepared with different surface charge densities and varying degrees of homogenization and their performance as binder for flexible LiFePO4 electrodes. The results show that the CNF with high charge density had shorter fiber lengths compared with those of CNF with low charge density, as observed with atomic force microscopy. Also, CNF processed with a large number of passes in the homogenizer showed a better fiber dispersibility, as observed from rheological measurements. The electrodes fabricated with highly charged CNF exhibited the best mechanical and electrochemical properties. The CNF at the highest charge density (ISSO mu mol g(-1)) and lowest degree of homogenization (3 + 3 passes in the homogenizer) achieved the overall best performance, including a high Young's modulus of approximately 311 MPa and a good rate capability with a stable specific capacity of 116 mAh g(-1) even up to 1 C. This work allows a better understanding of the influence of the processing parameters of CNF on their performance as binder for flexible electrodes. The results also contribute to the understanding of the optimal processing parameters of CNF to fabricate other materials, e.g., membranes or separators.

Place, publisher, year, edition, pages
2017. Vol. 9, no 43, p. 37712-37720
Keywords [en]
CNF, binder, charge density, degree of homogenization, flexible Li-ion batteries
National Category
Chemical Sciences
Research subject
Materials Chemistry
Identifiers
URN: urn:nbn:se:su:diva-150011DOI: 10.1021/acsami.7b10307ISI: 000414506600023PubMedID: 28972727OAI: oai:DiVA.org:su-150011DiVA, id: diva2:1167712
Available from: 2017-12-19 Created: 2017-12-19 Last updated: 2022-02-28Bibliographically approved
In thesis
1. Nanocellulose: Energy Applications and Self-Assembly
Open this publication in new window or tab >>Nanocellulose: Energy Applications and Self-Assembly
2019 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Technologies based on renewable materials are required to decrease the environmental cost and promote the development of a sustainable society. In this regard, nanocellulose extracted from wood finds many applications thanks to its intrinsic mechanical and chemical properties as well as the versatility in its manufacturing processes. In this thesis, I present the results of the investigations on carboxylated cellulose nanofibres (CNF) as ionic conductive membranes and electrode component in fuel cells and lithium ion batteries. Moreover, I also show the results of the assembly of CNF suspension and cellulose nanocrystals (CNC) - lepidocrocite nanorods (LpN) hybrids.

The fuel cell performance of CNF-based proton conductive membranes was evaluated as a function of intrinsic material parameters such as membrane thickness and surface charge density as well as extrinsic parameters such as the relative humidity (RH). It was found that the proton conductivity is about 2 mS cm-1 at 30 °C between 65 and 95 % RH. At the same time, the water uptake of the membrane was measured and correlated with the structural evolution of the membrane using small angle X-ray scattering.

The performance of the CNF-based separator in lithium ion batteries was investigated as a function of membrane porosity and protonation of the functional groups. The Li-ion battery assembled with the protonated separators showed stable and good rate performance.

The CNF was also tested as binder in lithium ion battery, showing that the morphology and mechanical properties of the cathode depend on the nanofibre surface charge and degree of defibrillation. In particular, high surface charge and medium degree of defibrillation give the best electrochemical performance.

Pyrolysed CNF (cCNF) improved the electrochemical performance of silicon nanoparticles-based anode thanks to the carbon network derived from the nanofibres. Si-cCNF has a capacity retention of 72.2 % after 500 cycles at 1 C and better performance rate than the pristine silicon nanoparticles.

Regarding the assembly of nanocellulose, the nematic order of CNF suspension at different nanofibre concentrations (0.5 – 4.9 wt%) was studied by small angle X-ray scattering, polarized optical microscopy and rheological measurements. The order parameter reaches a maximum value of 0.8 depending on the CNF concentration. Small angle neutron scattering with contrast matching experiments reveals that the natural alignment of CNC and LpN can be switched using a combination of magnetic fields of up to 6.8 T and varying the amount of LpN incorporated in the CNC.

Place, publisher, year, edition, pages
Stockholm: Department of Materials and Environmental Chemistry (MMK), Stockholm University, 2019. p. 82
Keywords
nanocellulose, self-assembly, fuel cell, lithium ion battery
National Category
Materials Chemistry
Research subject
Materials Chemistry
Identifiers
urn:nbn:se:su:diva-171459 (URN)978-91-7797-815-2 (ISBN)978-91-7797-816-9 (ISBN)
Public defence
2019-09-20, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockholm, 10:00 (English)
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Note

At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 1: Manuscript. Paper 6: Manuscript.

Available from: 2019-08-28 Created: 2019-08-08 Last updated: 2022-02-26Bibliographically approved

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Guccini, ValentinaSalazar-Alyarez, German

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