Volume 1 Issue 3
September  2022
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Junbo Wang, Sren L Dreyer, Kai Wang, Ziming Ding, Thomas Diemant, Guruprakash Karkera, Yanjiao Ma, Abhishek Sarkar, Bei Zhou, Mikhail V Gorbunov, Ahmad Omar, Daria Mikhailova, Volker Presser, Maximilian Fichtner, Horst Hahn, Torsten Brezesinski, Ben Breitung, Qingsong Wang. P2-type layered high-entropy oxides as sodium-ion cathode materials[J]. Materials Futures, 2022, 1(3): 035104. doi: 10.1088/2752-5724/ac8ab9
Citation: Junbo Wang, Sren L Dreyer, Kai Wang, Ziming Ding, Thomas Diemant, Guruprakash Karkera, Yanjiao Ma, Abhishek Sarkar, Bei Zhou, Mikhail V Gorbunov, Ahmad Omar, Daria Mikhailova, Volker Presser, Maximilian Fichtner, Horst Hahn, Torsten Brezesinski, Ben Breitung, Qingsong Wang. P2-type layered high-entropy oxides as sodium-ion cathode materials[J]. Materials Futures, 2022, 1(3): 035104. doi: 10.1088/2752-5724/ac8ab9
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P2-type layered high-entropy oxides as sodium-ion cathode materials

© 2022 The Author(s). Published by IOP Publishing Ltd on behalf of the Songshan Lake Materials Laboratory
Materials Futures, Volume 1, Number 3
  • Received Date: 2022-07-14
  • Accepted Date: 2022-08-18
  • Rev Recd Date: 2022-08-14
  • Publish Date: 2022-09-12
  • 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. Overall, the high-entropy strategy is a promising route for improving the electrochemical performance of P2 layered oxide cathodes for advanced sodium-ion battery applications.
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  • Conflict of interest

    There are no conflicts to declare.

    Author contributions

    J W, B B and Q W conceived the idea and designed the experiments. B B, H H and Q W supervised the project. S L D and T B conducted the DEMS measurements and analysed the data. K W and Z D performed the TEM measurements and analysed the data. T D, G K and M F collected the XPS spectra and analyzed the data. A S and Y M provided valuable suggestions during the whole project. B Z, M V G, A O and D M helped with the XAS measurements and analyzed the data. V P helped with the ICP-OES measurements. J W, B B and Q W prepared the initial manuscript. All authors discussed the results and contributed to discussion and reviewing the manuscript.

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