Publication date: 10th April 2024
Li metal solid state batteries (SSBs) enable high energy and power density and improve the overall safety of the device over conventional LiBs [1]. Removing the lithium metal anode solve critical problems ascribed to SSB manufacturing and increase the final energy density by optimizing the cell volume. In an anode-less battery, the Li-metal plates and strips on the bare current collector during cycling. The feasibility of this configuration in a SSB has already been demonstrated in several publications, although low coulombic efficiency and deeper understanding of interfaces are major challenges [2], [3], [4].
The aim here is to demonstrate the interfacial optimization of anode-less solid-state battery with Li7La3Zr2O12 (LLZO) electrolyte. Anode-less cells were assembled with various sputtered current collectors (CC) such as Cu and Ag. Cells with various Cu CC thicknesses were cycled to analyze electrodeposited Li morphology by post-mortem SEM analysis. Current collector and electrolyte surfaces were analyzed by Atomic force microscopy (AFM), Raman spectroscopy and Scanning electron microscopy (SEM), before and after cells cycling. Li nucleation and growth were further studied by Galvanostatic impedance spectroscopy (GEIS) to understand the complex nature of physical/chemical phenomena during in-situ plating of Li.
We found that Li nucleation potential is independent of CC thickness, however electrodeposited Li showed different morphology depending upon CC thickness. For the first time cells with Cu current collector and LLZO electrolyte worked up-to 100 cycles with a Cu layer as thin as 50nm and at very low nucleation potential of ~30mV. By addition of nanometric Ag interlayer in between LLZO and Cu, we could effectively control Li deposition [5]. The robust thin film interlayer enabled stable cycling, accommodating the volume changes without the need for extra external pressure.
As a part of the DESTINY PhD programme, this project received funding from the EU’s Horizon2020 research and innovation programme under the Marie Skłodowska Curie Actions COFUND (Grant Agreement#945357).
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