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Revealing the Atomic Origin of Heterogeneous Li‐Ion Diffusion by Probing Na
Author(s) -
Xiao Biwei,
Wang Kuan,
Xu GuiLiang,
Song Junhua,
Chen Zonghai,
Amine Khalil,
Reed David,
Sui Manling,
Sprenkle Vincent,
Ren Yang,
Yan Pengfei,
Li Xiaolin
Publication year - 2019
Publication title -
advanced materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.707
H-Index - 527
eISSN - 1521-4095
pISSN - 0935-9648
DOI - 10.1002/adma.201805889
Subject(s) - materials science , ion , atomic diffusion , atomic units , diffusion , cathode , chemical physics , valence (chemistry) , nanotechnology , chemistry , crystallography , thermodynamics , physics , organic chemistry , quantum mechanics
Abstract Tracing the dynamic process of Li‐ion transport at the atomic scale has long been attempted in solid state ionics and is essential for battery material engineering. Approaches via phase change, strain, and valence states of redox species have been developed to circumvent the technical challenge of direct imaging Li; however, all are limited by poor spatial resolution and weak correlation with state‐of‐charge (SOC). An ion‐exchange approach is adopted by sodiating the delithiated cathode and probing Na distribution to trace the Li deintercalation, which enables the visualization of heterogeneous Li‐ion diffusion down to the atomic level. In a model LiNi 1/3 Mn 1/3 Co 1/3 O 2 cathode, dislocation‐mediated ion diffusion is kinetically favorable at low SOC and planar diffusion along (003) layers dominates at high SOC. These processes work synergistically to determine the overall ion‐diffusion dynamics. The heterogeneous nature of ion diffusion in battery materials is unveiled and the role of defect engineering in tailoring ion‐transport kinetics is stressed.