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Moos, Ralf ; Hennerici, Lukas ; Sozak, Mutlucan ; Wiedemann, Kim ; Paulus, Daniel ; Schneider, Jürgen ; Donker, Nils ; Schönauer-Kamin, Daniela:
Producing Solid-State Batteries by the Powder Aerosol Deposition Method : Overview and Recent Progress.
2025
Veranstaltung: International Symposium on Green Processing for Advanced Ceramics - IGPAC 2025
, 5.10.-9.10.2025
, Ise-Shima/Mie, Japan.
(Veranstaltungsbeitrag: Kongress/Konferenz/Symposium/Tagung
,
Poster
)
Abstract
The Powder Aerosol Deposition Method (PAD or ADM) is a dry spray coating technique, that enables the production of dense ceramic films at room temperature. In this process, a ceramic powder is aerosolized in a gas stream and subsequently deposited onto a substrate inside a vacuum chamber. This process is particularly well suited for producing functional ceramic films. Notably, it finds applications in the development of dense lithium or sodium ion-conducting solid electrolyte membranes for solid-state batteries (SSB). Moreover, the powder aerosol deposition process can be used not only to produce membranes, but also to manufacture combinations of cathode films for intercalation as well as deintercalation reactions and ion-conducting membranes on a metal conductor. Consequently, it is possible to manufacture complete inorganic SSB architectures at room temperature without any inactive components such as binders. Several recent examples with respect to SSB are shown in this contribution. Lithium-based all-solid-state batteries (SSBs) are attracting worldwide attention as the next step in the evolution of Li-ion batteries (LIBs). They have the potential to resolve safety concerns and to increase the energy densities, which are key challenges for LIBs. The current focus is on enhancing the electrochemical properties of SSBs. However, a suitable economic method for fabricating them remains to be established, especially when ceramic materials are used as solid electrolytes. The powder aerosol deposition method is a ceramic processing method that uses raw ceramic powders to fabricate dense, several micrometer thick ceramic films.
Example 1: The garnet-like Li7La3Zr2O12 (LLZO) is a promising solid electrolyte (SE) for solid-state batteries (SSBs). The powder aerosol deposition method allows for the fabrication of dense LLZO films at room temperature. In this example, it is shown that aerosol deposited LLZO films can reversibly transport lithium up to at least 0.4 mA cm-2 without requiring a thermal post-treatment after deposition.
Example 2: The powder aerosol deposition method can be used to fabricate SSBs with LiNi0.83Mn0.11Co0.06O2 (NMC) as the cathode active material and Al0.2Li6.025La3Zr1.625Ta0.375O12 (LLZO) as the solid electrolyte. The cathode can be fabricated as a composite with a gradient in the electrolyte concentration. The successful fabrication is confirmed through scanning electron microscopy and energy-dispersive X-ray spectroscopy analysis. Electrochemical characterization shows that the obtained SSBs can be cycled. Furthermore, it can be shown that (at least) 145 μm thick NMC films can be fabricated by the powder aerosol deposition method. The electrochemical results are compared with the theoretical potential of all solid-state batteries, and methods to further improve the achieved state will be discussed. Due to the huge abundance of the element ‘‘sodium’’ in the Earth’s crust (~103 times more abundant compared to lithium), one may consider that Na-ion batteries open a new era of batteries in terms of their abundance, sustainability, and lower-cost.
Example 3: Therefore, Sodium (Na) Super-Ionic CONductor (NaSICON) solid electrolyte powders (Na3Zr2Si2PO12) were prepared by the mixed oxide technique using a planetary ball mill and synthesized via solid-state method at temperatures ranging from 950 to 1200 °C. The powders with 95% pure NaSICON phase were powder aerosol deposited on different substrates at room temperature directly from these powders. Fully dense ceramic films were obtained. XRD, including Rietveld refinement, was carried out on both the calcined powders and the resulting films to determine the crystallographic properties. The electrical properties of the resulting films were characterized and the effect of mild annealing between 100 and 600 °C on the ionic conductivity of the aerosol deposited NaSICON films was evaluated. The annealed films were electrically characterized in the temperature range between 50 °C and 250 °C. Despite the conductivity was two decades lower compared to the best values for bulk-NaSICON ceramic solids, it is assumed that the conductivity is still high enough, since dense powder aerosol deposited films feature thicknesses in the range of only 10 µm, which is promising for stationary energy storage applications of solid-state sodium batteries.
Example 4: In a subsequent study, it was shown that Na-based cathode composites of Na3V2(PO4)3/C (abbr. NVP/C) can be aerosol deposited on aluminum (Al) plates without any binder or solvent addition. As-deposited cathode composite films delivered a specific discharge capacity of almost 40 mAh/g, whereas after annealing even almost 65 mAh/g were reached. In this preliminary study, 20 cycles were applied at a C-Rate of C/10 with only a very slight degradation of discharge capacity. Moreover, it was revealed that the cathode active material (CAM) utilization is affected highly by the thickness of the aerosol deposited CAM films.
Example 5: A disadvantage when using NaSICON as the solid electrolyte is its poor wettability and electrochemical instability against a sodium metal anode. This causes interfacial challenges and may limit the practical application. Therefore, thin ceramic interlayers between NaSICON and the sodium metal anode could be integrated – of course, again using powder aerosol deposition. Two types of interlayer materials were investigated in this study: the insertion-type material rutile TiO2 and the conversion-type material CuO. Both interlayers were processed onto the bulk-NaSICON surface using powder aerosol deposition at room temperature. Dense, well-adhering ceramic interlayer films with approximate thicknesses of ~ 800 nm (rutile TiO2) and ~ 650 nm (CuO) were successfully deposited at room temperature. A critical current density of symmetric Na|NaSiCON|Na cells between 0.5 mA/cm² to over 4 mA/cm² (at 70 °C) was observed without interlayers. This is a well-known behavior and can be attributed to the instability of NaSICON against Na. Electrochemical impedance spectroscopy showed that the interfacial resistance increased from almost 3000 Ω to over 8000 Ω within ca. 3 weeks (stored at room temperature under open circuit conditions). The rutile TiO2 interlayer reduced the interfacial resistance by a factor of 3, but contact losses occurred during cycling, possibly due to changes of the crystal structure of the in-situ formed NaxTiO2 interphase. In contrast, CuO interlayers reduced the interfacial resistance by a factor of 6 and critical current density (CCD) values of almost 6 mA/cm² were achieved at 70 °C in the as-deposited state of the CuO interlayer and CCD values of almost 7.5 mA/cm² at 70 °C after thermal post-treatment of the aerosol deposited film were realized in the Na|CuO|NaSICON|CuO|Na configuration. This improvement is attributed to the in-situ formation of a porous, ionic/electronic conductive Na2O+Cu0 interphase. It supports stable sodium metal stripping and plating, reduces the interfacial resistance, and can even be further improved by thermal post-treatment. In summary, it can be stated that the powder aerosol deposition method offers many possibilities for producing both sodium and lithium ion-conducting films and even for manufacturing entire SSBs from them. While complete cells have already been produced for lithium-ion SSBs that have withstood multiple cycling, individual components for sodium-ion SSBs have been manufactured using the powder aerosol deposition method. hThis included both solid electrolyte layers and interfacial layers as well as composite cathodes.
Weitere Angaben
| Publikationsform: | Veranstaltungsbeitrag (Poster) |
|---|---|
| Begutachteter Beitrag: | Ja |
| Institutionen der Universität: | Fakultäten > Fakultät für Ingenieurwissenschaften Fakultäten > Fakultät für Ingenieurwissenschaften > Lehrstuhl Funktionsmaterialien > Lehrstuhl Funktionsmaterialien - Univ.-Prof. Dr.-Ing. Ralf Moos Profilfelder > Advanced Fields > Neue Materialien Forschungseinrichtungen > Zentrale wissenschaftliche Einrichtungen > Bayreuther Materialzentrum - BayMAT Forschungseinrichtungen > Zentrale wissenschaftliche Einrichtungen > Bayerisches Zentrum für Batterietechnik - BayBatt |
| Titel an der UBT entstanden: | Ja |
| Themengebiete aus DDC: | 600 Technik, Medizin, angewandte Wissenschaften > 620 Ingenieurwissenschaften |
| Eingestellt am: | 13 Okt 2025 07:02 |
| Letzte Änderung: | 13 Okt 2025 07:02 |
| URI: | https://eref.uni-bayreuth.de/id/eprint/94872 |