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High-Entropy Sulfides Catalyze Rate-Determining Redox in Fast-Charging Aqueous Zinc-Sulfur Batteries

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dc.contributor.authorLiu, J.
dc.contributor.authorWu, H.
dc.contributor.authorYe, C.
dc.contributor.authorQiao, S.
dc.date.issued2025
dc.description.abstractThe sluggish kinetics of the solid–solid Zn–S redox process significantly hinders the practical energy density and lifespan of fast-charging aqueous Zn–S batteries (AZSBs). Conventional low-entropy catalysts suffer from poor stability, leading to leaching effects and water splitting during cycling. To overcome these limitations, we present a three-step synthesis of high-entropy sulfide (HES) nanorod catalysts to accelerate the rate-determining step (RDS) in the Zn–S redox process. Operando synchrotron powder diffraction, operando synchrotron infrared reflectance microscopy, and operando Raman spectroscopy characterizations reveal that the HES catalysts improve sulfur utilization by accelerating the RDS conversion of ZnS₂ to wurtzite ZnS. Furthermore, near-edge X-ray absorption fine structure and inductively coupled plasma mass spectrometry analyses demonstrate that the HES catalysts effectively suppress the leaching effect of transition metals and water splitting of the aqueous electrolyte, improving cycling stability. In contrast, utilizing medium- and lowentropy catalysts results in the formation of by-products, including S₅ ²⁻, S₃ ²⁻, and SO₃ ²⁻ species. Consequently, the pouch cell with the HES catalysts delivers a high cathode energy density of 313 Wh kg⁻¹ and high cycling stability over 400 cycles at 4 C with 0.06% capacity decay per cycle. This entropy-driven catalytic strategy provides an effective approach for developing stable and fast-charging aqueous metal–sulfur batteries.
dc.description.statementofresponsibilityJiahao Liu, Han Wu, Chao Ye, and Shi-Zhang Qiao
dc.identifier.citationAngewandte Chemie International Edition, 2025; 64(28):e202503472-1-e202503472-8
dc.identifier.doi10.1002/anie.202503472
dc.identifier.issn1433-7851
dc.identifier.issn1521-3773
dc.identifier.orcidLiu, J. [0000-0002-7777-312X]
dc.identifier.orcidWu, H. [0000-0002-5281-7325]
dc.identifier.orcidQiao, S. [0000-0002-1220-1761] [0000-0002-4568-8422]
dc.identifier.urihttps://hdl.handle.net/2440/147321
dc.language.isoen
dc.publisherWiley
dc.relation.granthttp://purl.org/au-research/grants/arc/DE230101011
dc.relation.granthttp://purl.org/au-research/grants/arc/CE230100032
dc.relation.granthttp://purl.org/au-research/grants/arc/IL230100039
dc.relation.granthttp://purl.org/au-research/grants/arc/DP220102596
dc.rights© 2025 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
dc.source.urihttps://doi.org/10.1002/anie.202503472
dc.subjectFast-charging batteries; High-entropy catalysts; Rate-determining step; Zinc–sulfur batteries
dc.titleHigh-Entropy Sulfides Catalyze Rate-Determining Redox in Fast-Charging Aqueous Zinc-Sulfur Batteries
dc.typeJournal article
pubs.publication-statusPublished online

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