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나노입자 연구단
나노입자 연구단
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In Situ Tracking Kinetic Pathways of Li+/Na+ Substitution during Ion-Exchange Synthesis of LixNa1.5-xVOPO4F0.5

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Title
In Situ Tracking Kinetic Pathways of Li+/Na+ Substitution during Ion-Exchange Synthesis of LixNa1.5-xVOPO4F0.5
Author(s)
Park, YU; Bai, JM; Wang, LP; Gabin Yoon; Zhang, W; Kim, H; Lee, S; Kim, SW; Looney, JP; Kisuk Kang; Wang, F
Publication Date
2017-09
Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.139, no.36, pp.12504 - 12516
Publisher
AMER CHEMICAL SOC
Abstract
Ion exchange is a ubiquitous phenomenon central to wide industrial applications, ranging from traditional (bio)chemical separation to the emerging chimie douce synthesis of materials with metastable structure for batteries and other energy applications. The exchange process is complex, involving substitution and transport of different dons under non-equilibrium conditions, and thus difficult to probe, leaving a gap in mechanistic understanding of kinetic exchange pathways toward final products. Herein, we report in situ tracking kinetic pathways of Li+/Na+ substitution during solvothermal ion-exchange synthesis of LixNa1.5-xVOPO4F0.5 (0 <= x <= 1.5), a promising multi-Li polyanionic cathode for batteries. The real-time observation, corroborated by first-principles calculations, reveals a selective replacement of Na+ by Li+, leading to peculiar Na+/Li+/vacancy orderings in the intermediates. Contradicting the traditional belief of facile topotactic substitution via solid solution reaction, an abrupt two-phase transformation occurs and predominantly governs the kinetics of ion exchange and transport in the ID polyanionic framework, consequently leading to significant difference of Li stoichiometry and electrochemical properties in the exchanged products. The findings may help to pave the way for rational design of ion exchange synthesis for making new materials. © 2017 American Chemical Society
URI
https://pr.ibs.re.kr/handle/8788114/4230
ISSN
0002-7863
Appears in Collections:
Center for Nanoparticle Research(나노입자 연구단) > Journal Papers (저널논문)
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