Publication date: 10th April 2024
Rechargeable batteries can contribute to powering electric transportation and storing electrical energy generated from intermittent renewable sources. Li ion batteries (LIBs) are the current battery of choice and new types of batteries such as solid-state Li metal batteries (SSLMBs) are also under active research. There are constant demands for further improving rate capability and energy density of batteries. Thick electrodes can increase energy density at the cell level, but one of the limiting factors is slow ion transport kinetics that reduce capacity at increasing (dis)charge rates. This problem is exacerbated in SSLMBs as the ion transport coefficient is usually lower in solids than in liquids. Here, two novel processing technologies have been developed to optimise the battery electrode microstructure and improve ion diffusion kinetics: (i) directional ice templating (DIT) for fabricating thick (900 µm) cathodes with vertical pore arrays and porosity gradient for LIBs [1]; and (ii) directional freezing and polymerisation (DFP) for fabricating cathodes with vertical arrays of solid polymer electrolyte (SPE) directly incorporated in the cathode microstructure during processing for SSLMBs [2]. Both techniques reduced tortuosity τ of ion diffusion pathways through electrode thickness from ~3.3 for conventional electrodes to 1.5.
A new operando correlative imaging technique of combining X-ray Compton scattering imaging (XCS-I) and computed tomography (XCT) has also been developed that allows pixel-by-pixel mapping of Li+ chemical stoichiometry variations in a LiNi0.8Mn0.1Co0.1O2 composite cathode within a coin cell battery [3,4]. This technique shows how the anisotropic electrode microstructure improved Li+ ion diffusivity, homogenised Li+ ion concentrations, and improved energy storage performance.
This work is supported by the ERC Starting Grant (converted to UKRI funding EP/Y009908/1), the Faraday Institution research programme grants (FIRG060 and FIRG066), UKRI EPSRC UKRI Innovation Fellowship EP/S001239/1, EP/S001239/2, Faraday Institution Industry Fellowship FIIF015 and Imperial College London UKRI Impact Acceleration Account EP/X52556X/1.
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