Resolving the Role of Configurational Entropy in Improving Cycling Performance of Multicomponent Hexacyanoferrate Cathodes for Sodium-Ion Batteries

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Ma, Yanjiao ; Hu, Yang ; Pramudya, Yohanes ; Diemant, Thomas ; Wang, Qingsong ; Goonetilleke, Damian ; Tang, Yushu ; Zhou, Bei ; Hahn, Horst ; Wenzel, Wolfgang ; Fichtner, Maximilian ; Ma, Yuan ; Breitung, Ben ; Brezesinski, Torsten:
Resolving the Role of Configurational Entropy in Improving Cycling Performance of Multicomponent Hexacyanoferrate Cathodes for Sodium-Ion Batteries.
In: Advanced Functional Materials. Vol. 32 (2022) Issue 34 . - No. 2202372.
ISSN 1616-3028
DOI: https://doi.org/10.1002/adfm.202202372

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Abstract in another language

Abstract Mn-based hexacyanoferrate (Mn-HCF) cathodes for Na-ion batteries usually suffer from poor reversibility and capacity decay resulting from unfavorable phase transitions and structural degradation during cycling. To address this issue, the high-entropy concept is here applied to Mn-HCF materials, significantly improving the sodium storage capabilities of this system via a solid-solution mechanism with minor crystallographic changes upon de-/sodiation. Complementary structural, electrochemical, and computational characterization methods are used to compare the behavior of high-, medium-, and low-entropy multicomponent Mn-HCFs resolving, to our knowledge for the first time, the link between configurational entropy/compositional disorder (entropy-mediated suppression of phase transitions, etc.) and cycling performance/stability in this promising class of next-generation cathode materials.