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Controlling Interfacial Properties of Solid-State Lithium Batteries Using Atomic Layer Deposition

2018-12 , Joshi, Kirit

Solid-state lithium batteries (SSLiBs) could enable improved safety and higher energy density compared to traditional lithium-ion batteries due to the use of metal anodes without dendrite growth. However, successful implementation of solid electrolytes within batteries is contingent upon controlling the chemical, mechanical, and electronic properties at solid electrolyte/electrode interfaces. SSLiB interfaces can exhibit poor wetting properties, leading to interfacial void spaces and high impedance. Furthermore, many solid electrolytes are chemically unstable in contact with electrodes. This project aims to stabilize traditionally unstable interfaces between lithium metal and ceramic electrolytes through the use of atomic layer deposition (ALD) of thin film oxide protection layers. It is expected that these protection layers will improve wetting properties and prevent or slow detrimental anode-electrolyte interactions. A custom ALD instrument has been designed and constructed for this project. This fully-automated instrument allows for the deposition of ternary oxides with atomic precision. It features pneumatic control of valves, a custom LabVIEW Virtual Instrument interface, and real-time pressure feedback control. This instrument is ideal for coating nanometer-scale films on either bulk solid electrolyte pellets or on powder. The custom reactor is used to coat NASICON-type solid electrolytes, including Li1.4Al0.6Ge1.4(PO4)3 (LAGP), with oxide thin films (Al2O3, ZnO). These NASICON materials are shown to readily react in contact with Li metal. The effect of these ALD protection films on electrochemical behavior and lifetime are compared to that of uncoated materials to determine whether the ALD coating improves battery performance and stability. Ultrathin oxide layers are found to improve the stability of the solid electrolytes in contact with Li during galvanostatic cycling. In particular, the ALD layers are shown to substantially extend the time to failure during cycling and to alter degradation pathways within cells. In conjunction with other students, ex situ and in situ characterization is used to uncover the evolution of these layers during cycling. These results are important for the development of stabilized, high-conductivity solid electrolytes for solid-state batteries.