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p2-type layered high-entropy oxides as sodium-ion cathode materials

Materials Futures 2022年第3期1卷 171-184页

作者： 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 Institute of Nanotechnology Karlsruhe Institute of Technology(KIT)Hermann-von-Helmholtz-Platz 176344 Eggenstein-LeopoldshafenGermany Helmholtz Institute Ulm(HIU)Electrochemical Energy Storage Helmholtzstrasse 1189081 UlmGermany Joint Research Laboratory Nanomaterials-Technische Universität Darmstadt and Karlsruhe Institute of Technology(KIT) Otto-Berndt-Strasse 364206 DarmstadtGermany Leibniz Institute for Solid State and Materials Research(IFW)Dresden Helmholtzstrasse 2001069 DresdenGermany INM-Leibniz Institute for New Materials Campus D2266123 SaarbrückenGermany Department for Materials Science and Engineering Saarland UniversityCampus D2266123 SaarbrückenGermany Saarene Saarland Center for Energy Materials and SustainabilityCampus C4266123 SaarbrückenGermany Bavarian Center for Battery Technology(BayBatt) University of BayreuthUniversitätsstrasse 3095447 BayreuthGermany Department of Chemistry University of BayreuthUniversitätsstrasse 3095447 BayreuthGermany

p2-type layered oxides with the general Na-deficient composition Na_(x)TMO_(2)(x<1,TM:transition metal)are a promising class of cathode materials for sodium-ion batteries.The open Na+transport pathways present in the ... 详细信息

p2-type layered oxides with the general Na-deficient composition Na_(x)TMO_(2)(xpromising 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,Na_(0.67)(Mn_(0.55)Ni_(0.21)Co_(0.24))O_(2),Na_(0.67)(Mn_(0.45)Ni_(0.18)Co_(0.24)Ti_(0.1)Mg_(0.03))O_(2) and Na_(0.67)(Mn_(0.45)Ni_(0.18)Co_(0.18)Ti_(0.1)Mg_(0.03)Al_(0.04)Fe_(0.02))O_(2) 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.

关键词： p2-type layered cathode high-entropy oxides sodium-ion battery gassing behavior manganese leaching

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