Vadhva, Pooja;
Boyce, Adam M;
Hales, Alastair;
Pang, Mei-Chin;
Patel, Anisha N;
Shearing, Paul R;
Offer, Gregory;
(2022)
Towards Optimised Cell Design of Thin Film Silicon-Based Solid-State Batteries via Modelling and Experimental Characterisation.
Journal of The Electrochemical Society
, 169
(10)
, Article 100525. 10.1149/1945-7111/ac9552.
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Abstract
To realise the promise of solid-state batteries, negative electrode materials exhibiting large volumetric expansions, such as Li and Si, must be used. These volume changes can cause significant mechanical stresses and strains that affect cell performance and durability, however their role and nature in SSBs are poorly understood. Here, a 2D electro-chemo-mechanical model is constructed and experimentally validated using steady-state, transient and pulsed electrochemical methods. The model geometry is taken as a representative cross-section of a non-porous, thin-film solid-state battery with an amorphous Si (a-Si) negative electrode, lithium phosphorous oxynitride (LiPON) solid electrolyte and LiCoO2 (LCO) positive electrode. A viscoplastic model is used to predict the build-up of strains and plastic deformation of a-Si as a result of (de)lithiation during cycling. A suite of electrochemical tests, including electrochemical impedance spectroscopy, the galvanostatic intermittent titration technique and hybrid pulse power characterisation are carried out to establish key parameters for model validation. The validated model is used to explore the peak interfacial (a-Si∣LiPON) stress and strain as a function of the relative electrode thickness (up to a factor of 4), revealing a peak volumetric expansion from 69% to 104% during cycling at 1C. The validation of this electro-chemo-mechanical model under load and pulsed operating conditions will aid in the cell design and optimisation of solid-state battery technologies.
| Type: | Article |
|---|---|
| Title: | Towards Optimised Cell Design of Thin Film Silicon-Based Solid-State Batteries via Modelling and Experimental Characterisation |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1149/1945-7111/ac9552 |
| Publisher version: | https://doi.org/10.1149/1945-7111/ac9552 |
| Language: | English |
| Additional information: | © 2022 The Author(s). Published on behalf of The Electrochemical Society by IOP Publishing Limited. This is an open access article distributed under the terms of the Creative Commons Attribution 4.0 License (CC BY, http://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse of the work in any medium, provided the original work is properly cited. |
| UCL classification: | UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering UCL > Provost and Vice Provost Offices > UCL BEAMS UCL |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10158055 |
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