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Direct Observation of Alternating Octahedral and Prismatic Sodium Layers in O3-Type Transition Metal Oxides

Author(s)
Kim, Jae ChulKwon, Deok-HwangYang, Julia H.Kim, HyunchulBo, Shou-HangWu, LijunKim, HaegyeomSeo, Dong-HwaShi, TanWang, JingyangZhu, YimeiCeder, Gerbrand
Issued Date
2020-08
DOI
10.1002/aenm.202001151
URI
https://scholarworks.unist.ac.kr/handle/201301/47261
Fulltext
https://onlinelibrary.wiley.com/doi/full/10.1002/aenm.202001151
Citation
ADVANCED ENERGY MATERIALS, v.10, no.31, pp.2001151
Abstract
The oxygen stacking of O3-type layered sodium transition metal oxides (O3-NaTMO2) changes dynamically upon topotactic Na extraction and reinsertion. While the phase transition from octahedral to prismatic Na coordination that occurs at intermediate desodiation by transition metal slab gliding is well understood, the structural evolution at high desodiation, crucial to achieve high reversible capacity, remains mostly uncharted. In this work, the phase transitions of O3-type layered NaTMO(2)at high voltage are investigated by combining experimental and computational approaches. An OP2-type phase that consists of alternating octahedral and prismatic Na layers is directly observed by in situ X-ray diffraction and high-resolution scanning transmission electron microscopy. The origin of this peculiar phase is explained by atomic interactions involving Jahn-Teller active Fe(4+)and distortion tolerant Ti(4+)that stabilize the local Na environment. The path-dependent desodiation and resodiation pathways are also rationalized in this material through the different kinetics of the prismatic and octahedral layers, presenting a comprehensive picture about the structural stability of the layered materials upon Na intercalation.
Publisher
WILEY-V C H VERLAG GMBH
ISSN
1614-6832
Keyword (Author)
energy storagelayered structureNa-ion batteriesO3 structureOP2 structure
Keyword
CATHODE MATERIALSIONDIFFUSIONPHASEINTERCALATIONPERFORMANCESTABILITYP2-TYPEVOLTAGE

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