4.8 Article

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

Journal

ADVANCED FUNCTIONAL MATERIALS
Volume 32, Issue 34, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202202372

Keywords

high-entropy materials; manganese-based hexacyanoferrates; phase transitions; secondary batteries; sodium-ion cathodes

Funding

  1. EnABLES, project - European Union [730957]
  2. EPISTORE, project - European Union [101017709]
  3. KeraSolar project
  4. Carl Zeiss Foundation
  5. European Union [957189]
  6. China Scholarship Council (CSC)
  7. Karlsruhe Nano Micro Facility (KNMF, ), a Helmholtz research infrastructure at Karlsruhe Institute of Technology (KIT, )
  8. German Research Foundation (DFG) [390874152]
  9. Projekt DEAL

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In this study, the high-entropy concept is applied to Mn-HCF materials, significantly improving the cycling performance and stability of 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, 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.

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