Volume 1 Issue 3
September  2022
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Junbo Wang, Sören 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, Sören 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
  • Publish Date: 2022-09-12
doi: 10.1088/2752-5724/ac8ab9

  • 1 Institute of Nanotechnology, Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany

  • 2 Helmholtz Institute Ulm (HIU) Electrochemical Energy Storage, Helmholtzstrasse 11, 89081 Ulm, Germany

  • 3 Joint Research Laboratory Nanomaterials—Technische Universität Darmstadt and Karlsruhe Institute of Technology (KIT), Otto-Berndt-Strasse 3, 64206 Darmstadt, Germany

  • 4 Leibniz Institute for Solid State and Materials Research (IFW) Dresden, Helmholtzstrasse 20, 01069 Dresden, Germany

  • 5 INM—Leibniz Institute for New Materials, Campus D2 2, 66123 Saarbrücken, Germany

  • 6 Department for Materials Science and Engineering, Saarland University, Campus D2 2, 66123 Saarbrücken, Germany

  • 7 Saarene, Saarland Center for Energy Materials and Sustainability, Campus C4 2, 66123 Saarbrücken, Germany

Funds:

J W, K W, Z D and B Z acknowledge financial support from the China Scholarship Council (CSC). G K and M F gratefully acknowledge financial support by Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany’s Excellence Strategy, EXC 2154, project number 390874152. A O acknowledges financial support from the Federal Ministry of Education and Research (Bundesministerium für Bildung und Forschung, BMBF) under the project ‘KaSiLi’ (03XP0254D) in the competence cluster ‘ExcellBattMat’. H H, B B and T B acknowledge financial support from the Helmholtz Association (DigiBat project). Financial support by the German Research Foundation (to H H, Grant No. HA 1344/43-1) is gratefully acknowledged. Q W and B B acknowledge the support from EnABLES and EPISTORE, projects funded by the European Union’s Horizon 2020 research and innovation program under Grant Agreement No. 730957 and 101017709, respectively. B B also acknowledges funding from the Kera-Solar project (Carl Zeiss Foundation). Beamtime allocation and support at beamline P65 of the PETRA III synchrotron (Deutsches Elektronen-Synchrotron DESY, Hamburg, Germany) is gratefully acknowledged. The INM authors thank Eduard Arzt (INM) for his continuing support. The authors acknowledge Andrea Jung (INM) for her support on ICP-OES measurements. The authors further acknowledge the support from the Karlsruhe Nano Micro Facility (KNMF, www.knmf.kit.edu), a Helmholtz research infrastructure at Karlsruhe Institute of Technology (KIT, www.kit.du).

    Abstract

  • 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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