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Lithium containing layered high entropy oxide structures

  • Wang, Junbo1
  • Cui, Yanyan1
  • Wang, Qingsong1
  • Wang, Kai2
  • Huang, Xiaohui2
  • Stenzel, David1
  • Sarkar, Abhishek1, 3
  • Azmi, Raheleh1
  • Bergfeldt, Thomas1
  • Bhattacharya, Subramshu S.4
  • Kruk, Robert1
  • Hahn, Horst1, 3, 5
  • Schweidler, Simon1
  • Brezesinski, Torsten1
  • Breitung, Ben1
  • 1 Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, Eggenstein-Leopoldshafen, 76344, Germany , Eggenstein-Leopoldshafen (Germany)
  • 2 Technische Universität Darmstadt, Alarich-Weiss-Str. 2, Darmstadt, 64287, Germany , Darmstadt (Germany)
  • 3 Joint Research Laboratory Nanomaterials – Technische Universität Darmstadt and Karlsruhe Institute of Technology (KIT), Otto-Berndt-Str. 3, Darmstadt, 64206, Germany , Darmstadt (Germany)
  • 4 Indian Institute of Technology Madras, Chennai, 600036, India , Chennai (India)
  • 5 Helmholtz Institute Ulm for Electrochemical Energy Storage, Helmholtzstr. 11, Ulm, 89081, Germany , Ulm (Germany)
Published Article
Scientific Reports
Springer Nature
Publication Date
Oct 28, 2020
DOI: 10.1038/s41598-020-75134-1
Springer Nature


Layered Delafossite-type Lix(M1M2M3M4M5…Mn)O2 materials, a new class of high-entropy oxides, were synthesized by nebulized spray pyrolysis and subsequent high-temperature annealing. Various metal species (M = Ni, Co, Mn, Al, Fe, Zn, Cr, Ti, Zr, Cu) could be incorporated into this structure type, and in most cases, single-phase oxides were obtained. Delafossite structures are well known and the related materials are used in different fields of application, especially in electrochemical energy storage (e.g., LiNixCoyMnzO2 [NCM]). The transfer of the high-entropy concept to this type of materials and the successful structural replication enabled the preparation of novel compounds with unprecedented properties. Here, we report on the characterization of a series of Delafossite-type high-entropy oxides by means of TEM, SEM, XPS, ICP-OES, Mössbauer spectroscopy, XRD including Rietveld refinement analysis, SAED and STEM mapping and discuss about the role of entropy stabilization. Our experimental data indicate the formation of uniform solid-solution structures with some Li/M mixing.

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