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Overcoming the Obstacle of Polymer–Polymer Resistances in Double Layer Solid Polymer Electrolytes
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.ORCID iD: 0000-0002-3374-2276
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.ORCID iD: 0000-0002-9862-7375
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.ORCID iD: 0000-0002-8019-2801
2021 (English)In: The Journal of Physical Chemistry Letters, E-ISSN 1948-7185, Vol. 12, no 11, p. 2809-2814Article in journal (Refereed) Published
Abstract [en]

Double-layer solid polymer electrolytes (DLSPEs) comprising one layer that is stable toward lithium metal and one which is stable against a high-voltage cathode are commonly suggested as a promising strategy to achieve high-energy-density lithium batteries. Through in-depth EIS analysis, it is here concluded that the polymer–polymer interface is the primary contributor to electrolyte resistance in such DLSPEs consisting of polyether-, polyester-, or polycarbonate-bad SPEs. In comparison to the bulk ionic resistance, the polymer–polymer interface resistance is approximately 10-fold higher. Nevertheless, the interfacial resistance was successfully lowered by doubling the salt concentration from 25 to 50 wt % LiTFSI owing to improved miscibility at the interface of the two polymer layers.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2021. Vol. 12, no 11, p. 2809-2814
National Category
Materials Chemistry Polymer Chemistry
Research subject
Chemistry with specialization in Materials Chemistry; Chemistry with specialization in Polymer Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-440868DOI: 10.1021/acs.jpclett.1c00366ISI: 000635441500015PubMedID: 33710889OAI: oai:DiVA.org:uu-440868DiVA, id: diva2:1546227
Funder
EU, European Research Council, 771777Available from: 2021-04-21 Created: 2021-04-21 Last updated: 2024-07-04Bibliographically approved
In thesis
1. Exploring the Frontiers of Polymer Electrolytes for Battery Applications: From Surface to Bulk
Open this publication in new window or tab >>Exploring the Frontiers of Polymer Electrolytes for Battery Applications: From Surface to Bulk
2021 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Lithium-ion batteries have dominated the market since their inception in 1991 due to their unparalleled energy and power densities, but are now faced with new challenges. Growing demand for battery materials for energy intense applications and large-scale interim energy storage have emphasized the need for safe and sustainable battery electrolytes. In this context, non-flammable solid polymer electrolytes (SPEs) are a promising alternative to address the shortcomings of conventional liquid electrolytes. Despite its significance, little research has thus far been devoted to understanding the electrochemical stability of SPEs under the harsh conditions exerted by next-generation electrode materials.

In this thesis, the stability and ramifications of interfaces in polycarbonate- and polyester-based SPEs have been investigated. The polycarbonate exhibited severe degradation upon contact with lithium compared to its ester counterpart. Volatile species stemming from polycarbonate and salt decomposition were observed independent of irreversible current response, thus also highlighting the limitations of voltammetry techniques to determine the electrochemical stability. Two novel techniques were thus devised to evaluate electrochemical stability of SPEs under more realistic conditions. Characterization of the electrode−polyester interface revealed formation of highly resistive interfacial layers composed of polymer, salt and impurity derivatives. The emergence of a detrimental resistance emanating from the polymer−polymer interface was also observed, thus identifying a crucial hurdle for double-layer SPEs as a strategy to extend the stability window.

The application of polycarbonate/polyester-based polymer electrolytes for sodium-ion batteries was also studied. Sodium is far more abundant than lithium, and thereby an excellent chemistry platform to develop new sustainable battery materials. The polycarbonate exhibited an exceptional ability to dissolve large quantities of sodium salt without compromising the mechanical stability. Spectroscopic and thermal measurements revealed the emergence of an alternative ionic transport mechanism at concentrations within the polymer-in-salt regime, which was decoupled from the segmental motion of the polymer chains. By incorporating flexible polyester moieties in polycarbonates, an SPE with better transport properties compared to its individual subunits, and polyether counterparts, was obtained. Optimal salt concentration in this copolymer was dependent on the degree of crystallinity, determined by the portion of polyester. Finally, the practical application of these polymer electrolytes was demonstrated in solid-state sodium-ion batteries.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2021. p. 67
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 2044
Keywords
Lithium-ion batteries, solid-state polymer electrolytes, electrochemical stability window, interfaces, ionic conductivity, polycarbonate, polyester, sustainability, sodium-ion
National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-440905 (URN)978-91-513-1214-9 (ISBN)
Public defence
2021-06-11, Room Å2001, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 09:15 (English)
Opponent
Supervisors
Available from: 2021-05-19 Created: 2021-04-21 Last updated: 2021-06-23

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Sångeland, ChristoferMindemark, JonasBrandell, Daniel

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Sångeland, ChristoferTjessem, TrineMindemark, JonasBrandell, Daniel
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