Publication date: 10th April 2024
Thin layers have traditionally represented exceptional model systems for fundamental prospects in materials science. However, the extent of such an approach to be utilized in real devices e.g., for energy conversion and storage, is still limited. To date, one of the few successful examples of a commercial thin film energy device is the lithium solid-state battery (SSB) based on a lithium phosphorus oxynitride (LiPON) electrolyte. LiPON remains as the only option in this arena thanks to its stability towards Li-metal and low electronic conductivity. However, LiPON’s low ionic conductivity (c.a. 1 μS·cm-1) limits cells’ performance and its difficult processability hinders large-scale production. Among the alternative ceramic electrolytes, NASICON superionic solid electrolyte Li1+xAlxTi2-x(PO4)3 (LATP) is very promising due to its good ionic conductivity (c.a. 1 mS·cm-1) and stability in ambient air at high temperatures. Despite these advantages, all-ceramic devices based on LATP have not been reported, mainly due to interfacial reactivity between components.
In the present talk, we will present our latest advances in the implementation of thin films in ceramic SSBs and the development of novel investigation tools for materials research and device integration. With this aim, LATP and different electrode materials were deposited by Large-Area Pulsed Laser Deposition. Spinel LiMn2O4 and Li4Ti5O12, and olivine LiFePO4 were chosen, aiming to exploit their outstanding stability, low cost, and environmental friendliness. Bi-layers of LATP with these electrodes were fabricated in order to study the structure of the different interfaces. Various strategies such as the introduction of protective coatings or Rapid Thermal Processing (RTP) procedures are implemented with the aim of improving the quality of these electrode-electrolyte interfaces. The nature of such interfaces and their evolution after being subjected to electrochemical cycles has been examined from different perspectives applying a series of complementary techniques such as Focused Ion Beam-Secondary Ion Mass Spectroscopy (FIB-SIMS), Atom Probe Tomography (APT), Grazing Incidence Wide Angle X-Ray Scattering (GIWAXS), among others. Our results show the interface chemical stability and electrochemical performance of these bi-layers demonstrating their suitability for future thin-film solid state lithium batteries (SSLBs).
This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No 824072 (HARVESTORE), from the AfreeSSB project ) funded by the "Agencia Estatal de Investigación" through the M-ERA.NET program (PCI2022-132960), and from the “Generalitat de Catalunya” (2021 SGR 00750, NANOEN, and 2021 SGR 01286). J. C. G.- R. acknowledges the financial support provided by the European Union's Horizon 2020 research and innovation program under the Marie Skłodowska-Curie Grant Agreement No. 801342 (Tecniospring INDUSTRY), as well as by the Agency for Business Competitiveness of the Government of Catalonia.
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