Abstract

Thin-film batteries often contain oxides in the anode, cathode, and electrolyte materials. In-operando methods capable of Li and O depth profiling are relevant for battery research to study, e.g. diffusion and trapping of constituents. Here, we demonstrate ion beam–based analytical methods with high depth resolution and sensitivity for depth profiling Li and O in thin-film batteries using 10 MeV Li and He ions. Simultaneous depth profiling of Li and O was performed using combined coincidence elastic recoil detection analysis and Rutherford backscattering spectrometry measurements in the battery with 8 MeV He ions, and the Li and O transport was measured in operando. Reversible Li transport was observed from the LMO anode to the NbO cathode on charging and vice versa during discharging. O transport was observed from the LMO anode to the NbO cathode on first charging with 3.5 V but was not observed on further charging and discharging of the battery. Our in-operando measurements allow direct and quantitative observation of Li and O transport during charge-discharge cycles for thin-film batteries.

Highlights

  • Liquid electrolytes as used in conventional Li-batteries are potentially hazardous because of the growth of lithium dendrites in the batteries, which leads to shorting, as well as the fact that these electrolytes are highly flammable

  • Coincidence ERDA was performed by 10 MeV 4He2þ primary ions for comparison

  • Our results show coincidence ERDA can be used for simultaneous depth profiling of O and Li

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Summary

Introduction

Liquid electrolytes as used in conventional Li-batteries are potentially hazardous because of the growth of lithium dendrites in the batteries, which leads to shorting, as well as the fact that these electrolytes are highly flammable. For safety reasons, the use of Li metal in conventional batteries is limited [1]. All solid-state Li-ion batteries (ASSLB) are promising candidates for high density energy storage and wearable electronics which for safety reasons may outperform conventional Li-ion batteries which use a less stable liquid electrolyte [2]. Solid-state batteries may use electrolytes such as LieS [3], LieO [4], or Li-polymer [5]. We demonstrate simultaneous depth profiling of Li and O in a TFB stack by coincidence ERDA methods. We studied Li and O transport in the TFB by combining simultaneous measurements of coincidence ERDA and Rutherford backscattering spectrometry (RBS) during charge/ discharge cycles

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