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Synergy of cations in high entropy oxide lithium ion battery anode

Wang, Kai 1; Hua, Weibo 2; Huang, Xiaohui 1; Stenzel, David 1; Wang, Junbo 1; Ding, Ziming 1; Cui, Yanyan 1; Wang, Qingsong 1; Ehrenberg, Helmut 2; Breitung, Ben ORCID iD icon 1; Kübel, Christian ORCID iD icon 1,3,4; Mu, Xiaoke 1
1 Institut für Nanotechnologie (INT), Karlsruher Institut für Technologie (KIT)
2 Institut für Angewandte Materialien – Energiespeichersysteme (IAM-ESS), Karlsruher Institut für Technologie (KIT)
3 Helmholtz-Institut Ulm (HIU), Karlsruher Institut für Technologie (KIT)
4 Karlsruhe Nano Micro Facility (KNMF), Karlsruher Institut für Technologie (KIT)


High entropy oxides (HEOs) with chemically disordered multi-cation structure attract intensive interest as negative electrode materials for battery applications. The outstanding electrochemical performance has been attributed to the high-entropy stabilization and the so-called ‘cocktail effect’. However, the configurational entropy of the HEO, which is thermodynamically only metastable at room-temperature, is insufficient to drive the structural reversibility during conversion-type battery reaction, and the ‘cocktail effect’ has not been explained thus far. This work unveils the multi-cations synergy of the HEO Mg$_{0.2}$Co$_{0.2}$Ni$_{0.2}$Cu$_{0.2}$Zn$_{0.2}$O at atomic and nanoscale during electrochemical reaction and explains the ‘cocktail effect’. The more electronegative elements form an electrochemically inert 3-dimensional metallic nano-network enabling electron transport. The electrochemical inactive cation stabilizes an oxide nanophase, which is semi-coherent with the metallic phase and accommodates Li$^+$ ions. This self-assembled nanostructure enables stable cycling of micron-sized particles, which bypasses the need for nanoscale pre-modification required for conventional metal oxides in battery applications. ... mehr

Verlagsausgabe §
DOI: 10.5445/IR/1000157414
Veröffentlicht am 29.03.2023
DOI: 10.1038/s41467-023-37034-6
Zitationen: 72
Zitationen: 79
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Angewandte Materialien – Energiespeichersysteme (IAM-ESS)
Helmholtz-Institut Ulm (HIU)
Institut für Nanotechnologie (INT)
Karlsruhe Nano Micro Facility (KNMF)
Post Lithium Storage (POLiS)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2023
Sprache Englisch
Identifikator ISSN: 2041-1723
KITopen-ID: 1000157414
HGF-Programm 38.02.01 (POF IV, LK 01) Fundamentals and Materials
Weitere HGF-Programme 43.31.01 (POF IV, LK 01) Multifunctionality Molecular Design & Material Architecture
Erschienen in Nature Communications
Verlag Nature Research
Band 14
Seiten Art.-Nr.: 1487
Bemerkung zur Veröffentlichung Gefördert durch den KIT-Publikationsfonds
Vorab online veröffentlicht am 17.03.2023
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