首页|Identification of optimal composition with superior electrochemical properties along the zero Mn3+line in Na0.75(Mn-Al-Ni)O2 pseudo ternary system
Identification of optimal composition with superior electrochemical properties along the zero Mn3+line in Na0.75(Mn-Al-Ni)O2 pseudo ternary system
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Biphasic layered oxide cathodes,known for their superior electrochemical performance,are prime can-didates for commercializing in Na-ion batteries.Herein,we unveil a series of P3/P2 monophasic and biphasic Al-substituted Na3/4Mn5-x/8Al2x/8Ni3-x/8O2 layered oxide cathodes that lie along the'zero Mn3+line'in the Na3/4(Mn-AI-Ni)O2 pseudo-ternary system.The structural analysis showed a larger Na+conduction bottleneck area in both P3 and P2 structures with a higher Al3+content,which enhanced their rate per-formance.In each composition,the P3/P2 biphasic compound with nearly equal fractions of P3 and P2 phases outperformed their monophasic counterparts in almost all electrochemical performance param-eters.Operando synchrotron XRD measurements obtained for the monophasic P3 and biphasic P2/P3 samples revealed the absence of the O3 phase during cycling.The high structure stability and faster Na+transport kinetics in the biphasic samples underpins the enhancement of electrochemical properties in the Al-substituted P3/P2 cathodes.These results highlight fixed oxidation state lines as a novel tool to identify and design layered oxide cathodes for Na-ion batteries in pseudo-ternary diagrams involving Jahn-Teller active cations.