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

Mi Ru Jo, Yunok Kim, Junghoon Yang, Mihee Jeong, Kyeongse Song, Yong-Il Kim, Jin-Myoung Lim, Maenghyo Cho, Jae-Hyun Shim, Young-Min Kim, Won-Sub Yoon () and Yong-Mook Kang ()
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Mi Ru Jo: Dongguk University-Seoul
Yunok Kim: Sungkyunkwan University
Junghoon Yang: Dongguk University-Seoul
Mihee Jeong: Sungkyunkwan University
Kyeongse Song: Dongguk University-Seoul
Yong-Il Kim: Korea Research Institute of Standards and Science (KRISS)
Jin-Myoung Lim: Seoul National University
Maenghyo Cho: Seoul National University
Jae-Hyun Shim: Dongshin University
Young-Min Kim: Sungkyunkwan University
Won-Sub Yoon: Sungkyunkwan University
Yong-Mook Kang: Dongguk University-Seoul

Nature Communications, 2019, vol. 10, issue 1, 1-9

Abstract: 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.

Date: 2019
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DOI: 10.1038/s41467-019-11195-9

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