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Solid polymer electrolyte coating from a bifunctional monomer for three-dimensional microbattery applications
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.
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, Polymer Chemistry.
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2013 (English)In: Journal of Power Sources, ISSN 0378-7753, E-ISSN 1873-2755, Vol. 238, 435-441 p.Article in journal (Refereed) Published
Abstract [en]

This work comprises the synthesis and characterization of a novel solid polymer electrolyte based on oligomeric polyetheramine substituted with a methacrylic group at one of its three chain ends. This modification introduces a bifunctionality to the PEA monomer it can act both as polymerizable unit and surfactant. Thin and pinhole-free polymer electrolyte layers could be constructed with thicknesses in the order of <1 mu m using UV-initiated polymerization. The electrolyte exhibits good electrochemical and chemical stability up to 4 V vs. Li+/Li. LiFePO4 cathode coated with the electrolyte was cycled against lithium at 60 degrees C, and displayed reasonable capacity values (similar to 140 mAh g(-1)) for 10 cycles, where after Li dendrite formation contributed to battery instabilities. 

Place, publisher, year, edition, pages
2013. Vol. 238, 435-441 p.
Keyword [en]
3D-microbattery solid electrolyte, Polymer electrolyte, Bifunctional monomer, Polyetheramine
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:uu:diva-204760DOI: 10.1016/j.jpowsour.2013.04.058ISI: 000320901900058OAI: oai:DiVA.org:uu-204760DiVA: diva2:641171
Available from: 2013-08-15 Created: 2013-08-12 Last updated: 2017-12-06Bibliographically approved
In thesis
1. Fabrication of Polymer Electrolytes for 3D-Microbatteries
Open this publication in new window or tab >>Fabrication of Polymer Electrolytes for 3D-Microbatteries
2013 (English)Licentiate thesis, comprehensive summary (Other academic)
Abstract [en]

Pressing demands on electrical energy storage require high power and high energy density rechargeable batteries with improved safety, reliable performance and low cost. This has led to reconsiderations in the choice of battery chemistry and battery design. Practical concerns originating from the use of flammable liquid electrolytes has renewed the interests in using solvent-free polymer electrolytes as flexible solid ionic conductors. At the same time, the limitations of conventional planar battery designs have seen the utilization of these materials in novel battery designs, such as three-dimensional microbatteries (3DMBs).

In this work, solvent-free polymer electrolytes have been tailored for 3DMB applications, due to their beneficial properties of non-flammability and dimensional stability. Polymer electrolytes based on functionalized poly(propylene glycol) triamine (PEA)-based oligomer have been developed via different synthetic routes, their potential use in 3DMBs has been demonstrated, and also their applicability for batteries of conventional dimensions. By tailoring the functionality in PEA oligomer, the electrolyte can be self-assembled and in-situ polymerized onto semi-3D (e.g., LiFePO4 composite) and 3D electrodes (e.g., 3D Cu-nanopillar) using in-situ UV-initiated polymerization or electropolymerization. The obtained conformal and uniform coatings, with thicknesses down to micro- and nano-dimensions, display useful ionic conductivity and stability for 3DMB applications.

Moreover, high molecular weight poly(trimethylene carbonate) (PTMC), serving as a polymer host material alternative to the conventional polyethers, was investigated for Li-ion batteries and potential implementation in 3DMBs. Polymer electrolytes with useful electrochemical stability and flexibility have been tested in LiFePO4 half-cells and demonstrate promising cycling performance comparable to liquid electrolyte-based counterparts at elevated temperature. 

Place, publisher, year, edition, pages
Uppsala: Kph Trycksaksbolaget, 2013. 50 p.
Keyword
3D-microbattery, Polymer electrolyte, Multifunctional monomer, Polyetheramine, Polycarbonate
National Category
Chemical Sciences
Research subject
Chemistry with specialization in Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-208992 (URN)
Supervisors
Available from: 2013-10-16 Created: 2013-10-12 Last updated: 2013-10-16Bibliographically approved
2. Functional Polymer Electrolytes for Multidimensional All-Solid-State Lithium Batteries
Open this publication in new window or tab >>Functional Polymer Electrolytes for Multidimensional All-Solid-State Lithium Batteries
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Pressing demands for high power and high energy densities in novel electrical energy storage units have caused reconsiderations regarding both the choice of battery chemistry and design. Practical concerns originating in the conventional use of flammable liquid electrolytes have renewed the interests of using solvent-free polymer electrolytes (SPEs) as solid ionic conductors for safer batteries.

In this thesis work, SPEs developed from two polymer host structures, polyethers and polycarbonates, have been investigated for all-solid-state Li- and Li-ion battery applications. In the first part, functional polyether-based polymer electrolytes, such as poly(propylene glycol) triamine based oligomer and poly(propylene oxide)-based acrylates, were investigated for 3D-microbattery applications. The amine end-groups were favorable for forming conformal electrolyte coatings onto 3D electrodes via self-assembly. In-situ polymerization methods such as UV-initiated and electro-initiated polymerization techniques also showed potential to deposit uniform and conformal polymer coatings with thicknesses down to nano-dimensions.

Moreover, poly(trimethylene carbonate) (PTMC), an alternative to the commonly investigated polyether host materials, was synthesized for SPE applications and showed promising functionality as battery electrolyte. High-molecular-weight PTMC was first applied in LiFePO4-based batteries. By incorporating an oligomeric PTMC as an interfacial mediator, enhanced surface contacts at the electrode/SPE interfaces and obvious improvements in initial capacities were realized. In addition, room-temperature functionality of PTMC-based SPEs was explored through copolymerization of ε-caprolactone (CL) with TMC. Stable cycling performance at ambient temperatures was confirmed in P(TMC/CL)-based LiFePO4 half cells (e.g., around 80 and 150 mAh g-1 at 22 °C and 40 °C under C/20 rate, respectively). Through functionalization, hydroxyl-capped PTMC demonstrated good surface adhesion to metal oxides and was applied on non-planar electrodes. Ionic transport behavior in polycarbonate-SPEs was examined by both experimental and computational approaches. A coupling of Li ion transport with the polymer chain motions was demonstrated.

The final part of this work has been focused on exploring the key characteristics of the electrode/SPE interfacial chemistry using PEO and PTMC host materials, respectively. X-ray photoelectron spectroscopy (XPS) was used to get insights on the compositions of the interphase layers in both graphite and LiFePO4 half cells.  

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2015. 89 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1243
Keyword
Polymer electrolyte, Li-battery, 3D-microbattery, Functionalization, Polyether, Polycarbonate, Copolymer
National Category
Materials Chemistry
Research subject
Chemistry with specialization in Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-248084 (URN)978-91-554-9215-1 (ISBN)
Public defence
2015-05-22, Häggsalen, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 09:15 (English)
Opponent
Supervisors
Available from: 2015-04-28 Created: 2015-03-26 Last updated: 2015-07-07

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Sun, BingBowden, TimBrandell, Daniel

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