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P2-type layered high-entropy oxides as sodium-ion cathode materials

Wang, Junbo; Dreyer, Sören L.; Wang, Kai; Ding, Ziming; Diemant, Thomas; Karkera, Guruprakash; Ma, Yanjiao; Sarkar, Abhishek; Zhou, Bei; Gorbunov, Mikhail V.; Omar, Ahmad; Mikhailova, Daria; Presser, Volker; Fichtner, Maximilian 1; Hahn, Horst 2; Brezesinski, Torsten ORCID iD icon 2; Breitung, Ben ORCID iD icon 2; Wang, Qingsong
1 Helmholtz-Institut Ulm (HIU), Karlsruher Institut für Technologie (KIT)
2 Institut für Nanotechnologie (INT), Karlsruher Institut für Technologie (KIT)


P2-type layered oxides with the general Na-deficient composition NaxTMO2 (x < 1, TM: transition metal) are a promising class of cathode materials for sodium-ion batteries. The open Na+ transport pathways present in the structure lead to low diffusion barriers and enable high charge/discharge rates. However, a phase transition from P2 to O2 structure occurring above 4.2 V and metal dissolution at low potentials upon discharge results in rapid capacity degradation. In this work, we demonstrate the positive effect of configurational entropy on the stability of the crystal structure during battery operation. Three different compositions of layered P2-type oxides were synthesized by solid-state chemistry, Na0.67(Mn0.55Ni0.21Co0.24)O2, Na0.67(Mn0.45Ni0.18Co0.24Ti0.1Mg0.03)O2 and Na0.67(Mn0.45Ni0.18Co0.18Ti0.1Mg0.03Al0.04Fe0.02)O2 with low, medium and high configurational entropy, respectively. The high-entropy cathode material shows lower structural transformation and Mn dissolution upon cycling in a wide voltage range from 1.5 to 4.6 V. Advanced operando techniques and post-mortem analysis were used to probe the underlying reaction mechanism thoroughly. ... mehr

Verlagsausgabe §
DOI: 10.5445/IR/1000155709
Veröffentlicht am 07.02.2023
DOI: 10.1088/2752-5724/ac8ab9
Zitationen: 34
Zitationen: 34
Cover der Publikation
Zugehörige Institution(en) am KIT Helmholtz-Institut Ulm (HIU)
Institut für Nanotechnologie (INT)
Karlsruhe Nano Micro Facility (KNMF)
Post Lithium Storage (POLiS)
Publikationstyp Zeitschriftenaufsatz
Publikationsdatum 01.09.2022
Sprache Englisch
Identifikator ISSN: 2752-5724
KITopen-ID: 1000155709
HGF-Programm 43.31.02 (POF IV, LK 01) Devices and Applications
Weitere HGF-Programme 38.02.01 (POF IV, LK 01) Fundamentals and Materials
Erschienen in Materials Futures
Verlag Institute of Physics Publishing Ltd (IOP Publishing Ltd)
Band 1
Heft 3
Seiten Art.Nr. 035104
Schlagwörter 2021-027-031153 2022-028-031418 TEM
Nachgewiesen in Scopus
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