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Fabrication of Polymer Electrolytes for 3D-Microbatteries
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
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 [en]
3D-microbattery, Polymer electrolyte, Multifunctional monomer, Polyetheramine, Polycarbonate
National Category
Chemical Sciences
Research subject
Chemistry with specialization in Materials Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-208992OAI: oai:DiVA.org:uu-208992DiVA: diva2:655590
Supervisors
Available from: 2013-10-16 Created: 2013-10-12 Last updated: 2013-10-16Bibliographically approved
List of papers
1. Solid polymer electrolyte coating from a bifunctional monomer for three-dimensional microbattery applications
Open this publication in new window or tab >>Solid polymer electrolyte coating from a bifunctional monomer for three-dimensional microbattery applications
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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. 

Keyword
3D-microbattery solid electrolyte, Polymer electrolyte, Bifunctional monomer, Polyetheramine
National Category
Chemical Sciences
Identifiers
urn:nbn:se:uu:diva-204760 (URN)10.1016/j.jpowsour.2013.04.058 (DOI)000320901900058 ()
Available from: 2013-08-15 Created: 2013-08-12 Last updated: 2017-12-06Bibliographically approved
2. Polycarbonate-based solid polymer electrolytes for Li-ion batteries
Open this publication in new window or tab >>Polycarbonate-based solid polymer electrolytes for Li-ion batteries
2013 (English)In: Solid State Ionics, ISSN 0167-2738, E-ISSN 1872-7689, Vol. 262, 738-742 p.Article in journal (Refereed) Published
Abstract [en]

This paper reports the synthesis and application of high-molecular-weight poly(trimethylene carbonate) (PTMC) as a new host material for solid polymer electrolyte-based Li-ion batteries. PTMC was synthesized through bulk ring-opening polymerization of the cyclic monomer to yield a high-molecular-weight polymer to serve as a base material for the electrolytes. The thermal properties and ionic conductivity of polymer electrolytes with different salt ratios were measured by TGA/DSC and electrochemical impedance spectroscopy, respectively. The most conductive systems were found at [Li+]:[carbonate] ratios of 1:13 and 1:8, which showed electrochemical stability up to 5.0 V vs. Li/Li+ and an ionic conductivity on the order of 10− 7 Scm(-1) at 60 °C. LiFePO4 half-cells using the electrolytes demonstrated a plateau in the specific discharge capacity around 153 mAhg(-1) after long-term cycling. The functionality of the electrolytes for three-dimensional microbatteries was also confirmed.

Keyword
Polycarbonate; Trimethylene carbonate; Polymer electrolyte; Li-ion battery; 3D-microbattery
National Category
Chemical Sciences
Research subject
Chemistry
Identifiers
urn:nbn:se:uu:diva-208985 (URN)10.1016/j.ssi.2013.08.014 (DOI)000338810500161 ()
Conference
19th International Conference on Solid State Ionics (SSI), Kyoto, Japan, June 02-07, 2013
Available from: 2013-10-12 Created: 2013-10-12 Last updated: 2017-12-06Bibliographically approved
3. Electrochemical elaboration of electrodes and electrolytes for 3D structured batteries
Open this publication in new window or tab >>Electrochemical elaboration of electrodes and electrolytes for 3D structured batteries
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2013 (English)In: JOURNAL OF MATERIALS CHEMISTRY A, ISSN 2050-7488, Vol. 1, no 32, 9281-9293 p.Article in journal (Refereed) Published
Abstract [en]

The challenges associated with the fabrication of three-dimensional (3D) electrode and electrolyte materials for Li-ion batteries are discussed. The basic issues for achieving a solid 3D cell foundation, which can simultaneously offer sufficient electronic conductivity to enable stable cycling, as well as enough compatibility with the incorporation of complementary components, have been addressed. Various electrochemical strategies for elaborating such systems are discussed and critically examined. Several current collector systems are presented including electrochemically prepared Cu and Al nanorods and commercial aperiodic carbon structures. Further electrochemical coating approaches then provide a direct method for the deposition of thin layers of active materials successfully demonstrated here as coatings on both 3D metal structures and commercially available 3D-structured carbon substrates. Enhanced capacities per foot print area are demonstrated for a number of 3D electrode materials, namely polyaniline on reticulated vitreous carbon, Cu2O on copper nanorods and TiO2 on Al nanorods. The crucial points for achieving a thin conformal coating of the corresponding 3D electrode structures with solid polymer electrolytes are also carefully analysed and discussed. In this context electro-polymerisation is proposed as a viable route to form thin electrolyte layers with promising characteristics. The high versatility of electro-polymerisation in combination with the various structures and methodologies adopted here represents a further step towards the development of cost-effective 3D microbattery devices.

National Category
Natural Sciences
Identifiers
urn:nbn:se:uu:diva-207063 (URN)10.1039/c3ta11921a (DOI)000322121300036 ()
Available from: 2013-09-09 Created: 2013-09-09 Last updated: 2014-12-15

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