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Predicting lithium iron oxysulphides for battery cathodes

Zhu, B; Scanlon, DO; (2022) Predicting lithium iron oxysulphides for battery cathodes. ACS Applied Energy Materials , 5 (1) pp. 575-584. 10.1021/acsaem.1c03094. Green open access

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Cathode materials that have high specific energies and low manufacturing costs are vital for the scaling up of lithium-ion batteries (LIBs) as energy storage solutions. Fe-based intercalation cathodes are highly attractive because of the low cost and the abundance of raw materials. However, existing Fe-based materials, such as LiFePO4, suffer from low capacity due to the large size of the polyanions. Turning to mixed anion systems can be a promising strategy to achieve higher specific capacity. Recently, antiperovskite-structured oxysulfide Li2FeSO has been synthesized and reported to be electrochemically active. In this work, we perform an extensive computational search for iron-based oxysulfides using ab initio random structure searching (AIRSS). By performing an unbiased sampling of the Li–Fe–S–O chemical space, several oxysulfide phases have been discovered, which are predicted to be less than 50 meV/atom from the convex hull and potentially accessible for synthesis. Among the predicted phases, two anti-Ruddlesden–Popper-structured materials Li2Fe2S2O and Li4Fe3S3O2 have been found to be attractive as they have high theoretical capacities with calculated average voltages of 2.9 and 2.5 V, respectively, and their distances to hull are less than 5 meV/atom. By performing nudged-elastic band calculations, we show that the Li-ion transport in these materials takes place by hopping between the nearest neighboring sites with low activation barriers between 0.3 and 0.5 eV. The richness of materials yet to be synthesized in the Li–Fe–S–O phase field illustrates the great opportunity in these mixed anion systems for energy storage applications and beyond.

Type: Article
Title: Predicting lithium iron oxysulphides for battery cathodes
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/acsaem.1c03094
Publisher version: https://doi.org/10.1021/acsaem.1c03094
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher's terms and conditions.
Keywords: oxysulfides, battery cathodes, lithium-ion batteries, energy storage applications, crystal structure prediction, first-principles calculation
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10141152
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