Journal article

Publication year: 2023

Journal: Advanced Science

Volume number: 10

Issue number: 22

eISSN: 2198-3844

Open access status: Gold

DOI Link: https://doi.org/10.1002/advs.202302521

Publisher: Wiley

Abstract: 
Interfacial instability, viz., pore formation in the lithium metal anode (LMA) during discharge leading to high impedance, current focusing induced solid-electrolyte (SE) fracture during charging, and formation/behaviour of the solid-electrolyte interphase (SEI), at the anode, is one of the major hurdles in the development of solid-state batteries (SSBs). Also, understanding cell polarization behaviour at high current density is critical to achieving the goal of fast-charging battery and electric vehicle. Herein, via in situ electrochemical scanning electron microscopy (SEM) measurements, performed with freshly deposited lithium microelectrodes on transgranularly fractured fresh Li6PS5Cl (LPSCl), the Li|LPSCl interface kinetics are investigated beyond the linear regime. Even at relatively small overvoltages of a few mV, the Li|LPSCl interface shows non-linear kinetics. The interface kinetics possibly involve multiple rate-limiting processes, i.e., ion transport across the SEI and SE|SEI interfaces, as well as charge transfer across the Li|SEI interface. The total polarization resistance RP of the microelectrode interface is determined to be approximate to 0.8.. cm(2). It is further shown that the nanocrystalline lithium microstructure can lead to a stable Li|SE interface via Coble creep along with uniform stripping. Also, spatially resolved lithium deposition, i.e., at grain surface flaws, grain boundaries, and flaw-free surfaces, indicates exceptionally high mechanical endurance of flaw-free surfaces toward cathodic load (>150 mA cm(-2)). This highlights the prominent role of surface defects in dendrite growth.

Harvard Citation style: Singh, D., Fuchs, T., Krempaszky, C., Mogwitz, B. and Janek, J. (2023) Non-Linear Kinetics of The Lithium Metal Anode on Li6PS5Cl at High Current Density: Dendrite Growth and the Role of Lithium Microstructure on Creep, Advanced Science, 10(22), Article 2302521. https://doi.org/10.1002/advs.202302521

APA Citation style: Singh, D., Fuchs, T., Krempaszky, C., Mogwitz, B., & Janek, J. (2023). Non-Linear Kinetics of The Lithium Metal Anode on Li6PS5Cl at High Current Density: Dendrite Growth and the Role of Lithium Microstructure on Creep. Advanced Science. 10(22), Article 2302521. https://doi.org/10.1002/advs.202302521