Triggered reversible phase transformation between layered and spinel structure in manganese-based layered compounds.

Abstract:

:Irreversible phase transformation of layered structure into spinel structure is considered detrimental for most of the layered structure cathode materials. Here we report that this presumably irreversible phase transformation can be rendered to be reversible in sodium birnessite (NaxMnO2·yH2O) as a basic structural unit. This layered structure contains crystal water, which facilitates the formation of a metastable spinel-like phase and the unusual reversal back to layered structure. The mechanism of this phase reversibility was elucidated by combined soft and hard X-ray absorption spectroscopy with X-ray diffraction, corroborated by first-principle calculations and kinetics investigation. These results show that the reversibility, modulated by the crystal water content between the layered and spinel-like phases during the electrochemical reaction, could activate new cation sites, enhance ion diffusion kinetics and improve its structural stability. This work thus provides in-depth insights into the intercalating materials capable of reversible framework changes, thereby setting the precedent for alternative approaches to the development of cathode materials for next-generation rechargeable batteries.

journal_name

Nat Commun

journal_title

Nature communications

authors

Jo MR,Kim Y,Yang J,Jeong M,Song K,Kim YI,Lim JM,Cho M,Shim JH,Kim YM,Yoon WS,Kang YM

doi

10.1038/s41467-019-11195-9

subject

Has Abstract

pub_date

2019-09-02 00:00:00

pages

3385

issue

1

issn

2041-1723

pii

10.1038/s41467-019-11195-9

journal_volume

10

pub_type

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