Improved interface stability in NASICON-type solid Electrolytes with oxide and oxide-metal interlayers
Vikash Gajraj a, Kevin Castelló Lux a, Daiana Ferreira a, Olha Skurikhina a, Antonio Gianfranco Sabato a, Juan Carlos Gonzalez-Rosillo a, Alex Morata a, Albert Tarancón a
a Catalonia Institute for Energy Research, Jardins de les Dones de Negre 1, 2ª p., 08930, Barcelona, Spain
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
Advances in Li-Metal All-Solid-State Batteries: Processing, Manufacturing, and Integration - #AdvanceSSB
Sevilla, Spain, 2025 March 3rd - 7th
Organizer: Juan Carlos Gonzalez-Rosillo
Oral, Vikash Gajraj, presentation 202
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.202
Publication date: 16th December 2024

The performance of high energy density solid-state Li-metal batteries is typically also limited due to unstable interface between solid electrolytes and the Li metal. This is particularly critical when employing NASICON-based solid electrolytes, where the transition metal tends to reduce in the presence of Li-metal, together with the solid-electrolyte decomposition. In this work,  the interface stability of the Li1.3Al0.3Ti1.7(PO4)3 (LATP) and Li1.5Al0.5Ge1.5(PO4)3 (LAGP) with Lithium metal has been improved by coating of the electrolyte with binary metal oxides, such as Alumina and Zirconia, as a function of thickness  employing the atomic layer deposition (ALD) technique. Furthermore, our studies suggest that after coating the as deposited Alumina and Zirconia layer with specific metal, the assembled coin cells can run with low overpotentials and high stability even at medium current densities. For these studies, the coin cell CR2032 have been assembled in symmetrical mode (Li/interlayers/solid-electrolyte/interlayer/Li) and cycled with current density of 6.4, 12.8 and 25.6 μA cm-2 for 2 h platting and stripping conditions (50 cycles at each current density). Impedance studies also suggest an improved interface with low contact resistance before and even after the cycling at high current densities as compared to the pristine LATP as well as LAGP.  During this presentation, we will discuss the electrochemical performance of our surface-modified cells and present structural characterization to address the mechanisms for the observed improvements.

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