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Expansion-tolerant architectures for stable cycling of ultrahigh-loading sulfur cathodes in lithium-sulfur batteries

: Shaibani, Mahdokht; Mirshekarloo, Meysam Sharifzadeh; Singh, Ruhani; Easton, Christopher D.; Cooray, M.C. Dilusha; Eshraghi, Nicolas; Abendroth, Thomas; Dörfler, Susanne; Althues, Holger; Kaskel, Stefan; Hollenkamp, Anthony F.; Hill, Matthew R.; Majumder, Mainak

Fulltext ()

Science advances 6 (2020), No.1, Art. eaay2757
ISSN: 2375-2548
Journal Article, Electronic Publication
Fraunhofer IWS ()

Lithium-sulfur batteries can displace lithium-ion by delivering higher specific energy. Presently, however, the superior energy performance fades rapidly when the sulfur electrode is loaded to the required levels—5 to 10 mg cm−2— due to substantial volume change of lithiation/delithiation and the resultant stresses. Inspired by the classical approaches in particle agglomeration theories, we found an approach that places minimum amounts of a high-modulus binder between neighboring particles, leaving increased space for material expansion and ion diffusion. These expansion-tolerant electrodes with loadings up to 15 mg cm−2 yield high gravimetric (>1200 mA·hour g−1) and areal (19 mA·hour cm−2) capacities. The cells are stable for more than 200 cycles, unprecedented in such thick cathodes, with Coulombic efficiency above 99%.