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Mareike Wolter
Fraunhofer-Institut für Keramische Technologien und Systeme IKTS, Winterbergstr. 28, 01277 Dresden, Germany

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Journal article
Published: 03 February 2021 in Batteries
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We report a new process technique for electrode manufacturing for all solid-state batteries. Porous electrodes are manufactured by a tape casting process and subsequently infiltrated by a plastic crystal polymer electrolyte (PCPE). With a following isostatic lamination process, the PCPE was further integrated deeply into the porous electrode layer, forming a composite electrode. The PCPE comprises the plastic crystal succinonitrile (SN), lithium conductive salt LiTFSI and polyacrylonitrile (PAN) and exhibits suitable thermal, rheological (ƞ = 0.6 Pa s @ 80 °C 1 s−1) and electrochemical properties (σ > 10−4 S/cm @ 45 °C). We detected a lowered porosity of infiltrated and laminated electrodes through Hg porosimetry, showing a reduction from 25.6% to 2.6% (NCM infiltrated to laminated) and 32.9% to 4.0% (LTO infiltrated to laminated). Infiltration of PCPE into the electrodes was further verified by FESEM images and EDS mapping of sulfur content of the conductive salt. Cycling tests of full cells with NCM and LTO electrodes with PCPE separator at 45 °C showed up to 165 mAh/g at 0.03C over 20 cycles, which is about 97% of the total usable LTO capacity with a coulomb efficiency of between 98 and 99%. Cycling tests at 0.1C showed a capacity of ~128 mAh/g after 40 cycles. The C-rate of 0.2C showed a mean capacity of 127 mAh/g. In summary, we could manufacture full cells using a plastic crystal polymer electrolyte suitable for NCM and LTO active material, which is easily to be integrated into porous electrodes and which is being able to be used in future cell concepts like bipolar stacked cells.

ACS Style

Matthias Coeler; Vanessa Van Laack; Frederieke Langer; Annegret Potthoff; Sören Höhn; Sebastian Reuber; Katharina Koscheck; Mareike Wolter. Infiltrated and Isostatic Laminated NCM and LTO Electrodes with Plastic Crystal Electrolyte Based on Succinonitrile for Lithium-Ion Solid State Batteries. Batteries 2021, 7, 11 .

AMA Style

Matthias Coeler, Vanessa Van Laack, Frederieke Langer, Annegret Potthoff, Sören Höhn, Sebastian Reuber, Katharina Koscheck, Mareike Wolter. Infiltrated and Isostatic Laminated NCM and LTO Electrodes with Plastic Crystal Electrolyte Based on Succinonitrile for Lithium-Ion Solid State Batteries. Batteries. 2021; 7 (1):11.

Chicago/Turabian Style

Matthias Coeler; Vanessa Van Laack; Frederieke Langer; Annegret Potthoff; Sören Höhn; Sebastian Reuber; Katharina Koscheck; Mareike Wolter. 2021. "Infiltrated and Isostatic Laminated NCM and LTO Electrodes with Plastic Crystal Electrolyte Based on Succinonitrile for Lithium-Ion Solid State Batteries." Batteries 7, no. 1: 11.

Journal article
Published: 08 December 2020 in Batteries
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A hermetic dense polymer-carbon composite-based current collector foil (PCCF) for lithium-ion battery applications was developed and evaluated in comparison to state-of-the-art aluminum (Al) foil collector. Water-processed LiNi0.5Mn1.5O4 (LMNO) cathode and Li4Ti5O12 (LTO) anode coatings with the integration of a thin carbon primer at the interface to the collector were prepared. Despite the fact that the laboratory manufactured PCCF shows a much higher film thickness of 55 µm compared to Al foil of 19 µm, the electrode resistance was measured to be by a factor of 5 lower compared to the Al collector, which was attributed to the low contact resistance between PCCF, carbon primer and electrode microstructure. The PCCF-C-primer collector shows a sufficient voltage stability up to 5 V vs. Li/Li+ and a negligible Li-intercalation loss into the carbon primer. Electrochemical cell tests demonstrate the applicability of the developed PCCF for LMNO and LTO electrodes, with no disadvantage compared to state-of-the-art Al collector. Due to a 50% lower material density, the lightweight and hermetic dense PCCF polymer collector offers the possibility to significantly decrease the mass loading of the collector in battery cells, which can be of special interest for bipolar battery architectures.

ACS Style

Marco Fritsch; Matthias Coeler; Karina Kunz; Beate Krause; Peter Marcinkowski; Petra Pötschke; Mareike Wolter; Alexander Michaelis. Lightweight Polymer-Carbon Composite Current Collector for Lithium-Ion Batteries. Batteries 2020, 6, 60 .

AMA Style

Marco Fritsch, Matthias Coeler, Karina Kunz, Beate Krause, Peter Marcinkowski, Petra Pötschke, Mareike Wolter, Alexander Michaelis. Lightweight Polymer-Carbon Composite Current Collector for Lithium-Ion Batteries. Batteries. 2020; 6 (4):60.

Chicago/Turabian Style

Marco Fritsch; Matthias Coeler; Karina Kunz; Beate Krause; Peter Marcinkowski; Petra Pötschke; Mareike Wolter; Alexander Michaelis. 2020. "Lightweight Polymer-Carbon Composite Current Collector for Lithium-Ion Batteries." Batteries 6, no. 4: 60.

Journal article
Published: 30 July 2020 in Polymers
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Solid polymer electrolytes for bipolar lithium ion batteries requiring electrochemical stability of 4.5 V vs. Li/Li+ are presented. Thus, imidazolium-containing poly(ionic liquid) (PIL) networks were prepared by crosslinking UV-photopolymerization in an in situ approach (i.e., to allow preparation directly on the electrodes used). The crosslinks in the network improve the mechanical stability of the samples, as indicated by the free-standing nature of the materials and temperature-dependent rheology measurements. The averaged mesh size calculated from rheologoical measurements varied between 1.66 nm with 10 mol% crosslinker and 4.35 nm without crosslinker. The chemical structure of the ionic liquid (IL) monomers in the network was varied to achieve the highest possible ionic conductivity. The systematic variation in three series with a number of new IL monomers offers a direct comparison of samples obtained under comparable conditions. The ionic conductivity of generation II and III PIL networks was improved by three orders of magnitude, to the range of 7.1 × 10−6 Scm−1 at 20 °C and 2.3 × 10−4 Scm−1 at 80 °C, compared to known poly(vinylimidazolium·TFSI) materials (generation I). The transition from linear homopolymers to networks reduces the ionic conductivity by about one order of magnitude, but allows free-standing films instead of sticky materials. The PIL networks have a much higher voltage stability than PEO with the same amount and type of conducting salt, lithium bis(trifluoromethane sulfonyl)imide (LiTFSI). GII-PIL networks are electrochemically stable up to a potential of 4.7 V vs. Li/Li+, which is crucial for a potential application as a solid electrolyte. Cycling (cyclovoltammetry and lithium plating-stripping) experiments revealed that it is possible to conduct lithium ions through the GII-polymer networks at low currents. We concluded that the synthesized PIL networks represent suitable candidates for solid-state electrolytes in lithium ion batteries or solid-state batteries.

ACS Style

Eike T. Röchow; Matthias Coeler; Doris Pospiech; Oliver Kobsch; Elizaveta Mechtaeva; Roland Vogel; Brigitte Voit; Kristian Nikolowski; Mareike Wolter. In Situ Preparation of Crosslinked Polymer Electrolytes for Lithium Ion Batteries: A Comparison of Monomer Systems. Polymers 2020, 12, 1707 .

AMA Style

Eike T. Röchow, Matthias Coeler, Doris Pospiech, Oliver Kobsch, Elizaveta Mechtaeva, Roland Vogel, Brigitte Voit, Kristian Nikolowski, Mareike Wolter. In Situ Preparation of Crosslinked Polymer Electrolytes for Lithium Ion Batteries: A Comparison of Monomer Systems. Polymers. 2020; 12 (8):1707.

Chicago/Turabian Style

Eike T. Röchow; Matthias Coeler; Doris Pospiech; Oliver Kobsch; Elizaveta Mechtaeva; Roland Vogel; Brigitte Voit; Kristian Nikolowski; Mareike Wolter. 2020. "In Situ Preparation of Crosslinked Polymer Electrolytes for Lithium Ion Batteries: A Comparison of Monomer Systems." Polymers 12, no. 8: 1707.

Articles
Published: 08 November 2019 in Journal of Adhesion Science and Technology
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Filling of cells with liquid electrolytes is the time-determining step in the production of lithium-ion batteries (LIBs). The influencing factors are not completely understood and need further research. The adhesion of the solid components, i.e. anode, cathode and separators, to the electrolyte and the respective interfaces play an important role. In this study, the penetration of liquid electrolytes is monitored by a combination of tensiometry and chronoamperometry. A setup including all battery components is proposed as model for battery cells. Diethyl carbonate is employed as model for the electrolyte. The penetration rates of the liquid into a stepwise extended model setup (separator; anode; cathode; separator/anode; separator/cathode; and anode/separator/cathode) in confined geometry between glass plates are determined with reproducible results. A modified Washburn equation combining surface tensions of liquid and solids forming the interface, and complex geometries of separators and electrodes is used to develop the penetration model. Comparative measurements in a glove box yield comparable results with the real electrolyte solution. The penetration of the model electrolyte into ceramic-coated separators is significantly faster than into polyolefin separators due to higher surface roughness and higher polarity of ceramic-coated separators. The wetting times obtained by chronoamperometric measurements correlate with the tensiometric penetration rates. The higher the tensiometric penetration rate, the lower is the chronoamperometric wetting time. The results of the study contribute to a deeper understanding of the interactions between electrolyte and solid components in LIBs and provide a new method to pre-evaluate battery components.

ACS Style

Sebastian Beyer; Oliver Kobsch; Doris Pospiech; Frank Simon; Christian Peter; Kristian Nikolowski; Mareike Wolter; Brigitte Voit. Influence of surface characteristics on the penetration rate of electrolytes into model cells for lithium ion batteries. Journal of Adhesion Science and Technology 2019, 34, 849 -866.

AMA Style

Sebastian Beyer, Oliver Kobsch, Doris Pospiech, Frank Simon, Christian Peter, Kristian Nikolowski, Mareike Wolter, Brigitte Voit. Influence of surface characteristics on the penetration rate of electrolytes into model cells for lithium ion batteries. Journal of Adhesion Science and Technology. 2019; 34 (8):849-866.

Chicago/Turabian Style

Sebastian Beyer; Oliver Kobsch; Doris Pospiech; Frank Simon; Christian Peter; Kristian Nikolowski; Mareike Wolter; Brigitte Voit. 2019. "Influence of surface characteristics on the penetration rate of electrolytes into model cells for lithium ion batteries." Journal of Adhesion Science and Technology 34, no. 8: 849-866.