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ε-Caprolactone-based solid polymer electrolytes for lithium-ion batteries: synthesis, electrochemical characterization and mechanical stabilization by block copolymerization
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry.ORCID iD: 0000-0002-3009-8884
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.ORCID iD: 0000-0002-0366-7228
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
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2018 (English)In: RSC Advances, ISSN 2046-2069, E-ISSN 2046-2069, Vol. 8, no 30, p. 16716-16725Article in journal (Refereed) Published
Abstract [en]

In this work, three types of polymers based on epsilon-caprolactone have been synthesized: poly(epsilon-caprolactone), polystyrene-poly(epsilon-caprolactone), and polystyrene-poly(epsilon-caprolactone-r-trimethylene carbonate) (SCT), where the polystyrene block was introduced to improve the electrochemical and mechanical performance of the material. Solid polymer electrolytes (SPEs) were produced by blending the polymers with 10-40 wt% lithium bis(trifluoromethane) sulfonimide (LiTFSI). Battery devices were thereafter constructed to evaluate the cycling performance. The best performing battery half-cell utilized an SPE consisting of SCT and 17 wt% LiTFSI as both binder and electrolyte; a Li vertical bar SPE vertical bar LiFePO4 cell that cycled at 40 degrees C gave a discharge capacity of about 140 mA h g(-1) at C/5 for 100 cycles, which was superior to the other investigated electrolytes. Dynamic mechanical analysis (DMA) showed that the storage modulus E' was about 5 MPa for this electrolyte.

Place, publisher, year, edition, pages
2018. Vol. 8, no 30, p. 16716-16725
National Category
Polymer Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-340854DOI: 10.1039/c8ra00377gISI: 000431814500034OAI: oai:DiVA.org:uu-340854DiVA, id: diva2:1180066
Funder
Swedish Energy Agency, 42031-1EU, Horizon 2020, 685716Available from: 2018-02-04 Created: 2018-02-04 Last updated: 2018-08-27Bibliographically approved
In thesis
1. Block Copolymer Electrolytes: Polymers for Solid-State Lithium Batteries
Open this publication in new window or tab >>Block Copolymer Electrolytes: Polymers for Solid-State Lithium Batteries
2018 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The use of solid polymer electrolytes (SPEs) for lithium battery devices is a rapidly growing research area. The liquid electrolytes that are used today are inflammable and harmful towards the battery components. The adoption of SPEs could drastically improve this situation, but they still suffer from a too low performance at ambient temperatures for most practical applications. However, by increasing the operating temperature to between 60 °C and 90 °C, the electrolyte performance can be drastically increased. The drawback of this approach, partly, is that parasitic side reactions become noticeable at these elevated temperatures, thus affecting battery lifetime and performance. Furthermore, the ionically conductive polymer loses its mechanical integrity, thus triggering a need for an external separator in the battery device.

One way of combining both mechanical properties and electrochemical performance is to design block copolymer (BCP) electrolytes, that is, polymers that are tailored to combine one ionic conductive block with a mechanical block, into one polymer. The hypothesis is that the BCP electrolytes should self-assemble into well-defined microphase separated regions in order to maximize the block properties. By varying monomer composition and structure of the BCP, it is possible to design electrolytes with different battery device performance. In Paper I and Paper II two types of methacrylate-based triblock copolymers with different mechanical blocks were synthesized, in order to evaluate morphology, electrochemical performance, and battery performance. In Paper III and Paper IV a different strategy was adopted, with a focus on diblock copolymers. In this strategy, the ethylene oxide was replaced by poly(e-caprolactone) and poly(trimethylene carbonate) as the lithium-ion dissolving group. The investigated mechanical blocks in these studies were poly(benzyl methacrylate) and polystyrene. The battery performance for these electrolytes was superior to the methacrylate-based battery devices, thus resulting in stable battery cycling at 40 °C and 30 °C.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2018. p. 68
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1630
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:uu:diva-340856 (URN)978-91-513-0233-1 (ISBN)
Public defence
2018-03-23, Häggsalen, Ångströmlaboratoriet, Uppsala, 09:00 (English)
Opponent
Supervisors
Funder
Swedish Research Council
Available from: 2018-02-28 Created: 2018-02-04 Last updated: 2018-04-03

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Bergfelt, AndreasLacey, Matthew J.Hedman, JonasBrandell, DanielBowden, Tim

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