Insights on Solid-electrolyte/electrode interfaces of All-solid-state Batteries: Multiscale Framework

The harmonious transition of society towards carbon-free technologies, from fossil fuel to renewable energy sources only, including transition from combustion engined cars to electrical vehicles, requires efficient and safe energy storage technologies [1-3]. Among the various battery technologies being available today, all-solid-state batteries (ASSBs) have garnered a lot of attention, due to their many advantages, including the high thermal stability, non-flammability, long lifetime. Moreover, they enable the use of lithium metal anode (theoretical specific capacity 3862 mAh g-1), which would increase considerably the performance of the ASSBs [4,5]. However, the realization of ASSBs is hampered by a limited understanding of the nanometer-thin solid-state electrolyte/electrode buried interfaces. In this talk, we present our recent findings and theoretical developments on the nanometer-thin solid-state electrolyte and electrode interfaces of solid state electrolyte in combination with different anode and cathode electrode interfaces. By combining a multiscale framework (DFT, reactive force field to continuum scale) with surfaces and electrochemical techniques (including Electrochemical Impedance Spectroscopy), the structural origin of interfacial resistance, the degradation mechanisms, and the lithium-ion transport mechanism at the cathode interfaces at different working/environmental conditions (Electric field, temperature, state of charge, etc.) are now better understood. As a result, the strategy of a hybrid multiscale experimental and computational framework paves the way towards further understanding and (re-)designing highly compatible and stable

electrolyte/electrode interfaces, which can be extended to other energy conversion and storage devices. Some of the findings will be discussed during the presentation.

References

1. K. Dahal, et al., Sustain. Cities and Soc., 2018, 40, 222.

2. V. Stamenkovic, et al., Nat. Mater., 2017, 16, 57.

3. M. Whittingham, MRS Bull., 2008.

4. K. Takada, et al., ACS Energy Lett., 2018, 3, 98.

5. A. Zhamu, et al., Energy Environ. Sci., 2012, 5, 5701.