Abstract
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.
Highlights
Lithium-ion batteries have shown great application potential for mobile high-energy and fast charging devices, which, require a high current input and output [1,2]
Porous electrodes are manufactured by a tape casting process and subsequently infiltrated by a plastic crystal polymer electrolyte (PCPE)
Infiltration of PCPE into the electrodes was further verified by field emission scanning electron microscope (FESEM) images and EDS mapping of sulfur content of the conductive salt
Summary
Lithium-ion batteries have shown great application potential for mobile high-energy and fast charging devices (e.g., for cell phones or electric vehicles), which, require a high current input and output [1,2]. There are two main techniques for manufacturing of an electrode combined with a solid-state or polymer-based electrolyte: One option for fabrication is an infiltration-based process (infiltration electrode) It uses a conventional casted and dried porous electrode or membrane which is infiltrated with the solid-state electrolyte phase to fill the open porosity and forming a lithium conductive network in the electrode [22,23,24,25]. A disadvantage could be, that pores remain not infiltrated, if they are not accessible for the electrolyte and the full capacity of the electrode might not be reached Another option is a slurry-based process (composite electrode), in which all components (e.g., active particles, conductive carbon, binder and solid-state electrolyte) are dispensed in a solvent (e.g., NMP) and coated onto a current collector foil [26]. The C-rate performance from 0.03C up to 0.5C was characterized
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