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

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, sign...

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Bibliographic Details
Published in:Advanced functional materials 2022-08, Vol.32 (34), p.n/a
Main Authors: 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
Format: Article
Language:English
Subjects:
Cathodes
Crystallography
Cycles
Electrochemical analysis
Electrode materials
Entropy
high‐entropy materials
manganese‐based hexacyanoferrates
Materials science
Phase transitions
Rechargeable batteries
secondary batteries
Sodium
Sodium-ion batteries
sodium‐ion cathodes
Structural analysis
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Summary: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. A multicomponent hexacyanoferrate, NaxMn0.4Fe0.15Ni0.15Cu0.15Co0.15[Fe(CN)6]y, has been developed as a robust cathode active material for Na‐ion battery applications. Systematic comparison of the structural and chemical properties of high‐, medium‐, and low‐entropy Mn‐based hexacyanoferrates uncovers the origin of the improved cycling performance, namely entropy‐mediated suppression of side reactions and phase transitions.
ISSN:1616-301X
1616-3028
DOI:10.1002/adfm.202202372