Journal
ADVANCED MATERIALS
Volume 31, Issue 29, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201805889
Keywords
dislocation diffusion; ion exchange; layer diffusion; layered cathodes; lithium-ion batteries
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Funding
- U.S. Department of Energy's (DOE's) Office of Electricity Delivery and Energy Reliability (OE) [70247A]
- U.S. Department of Energy (DOE), Vehicle Technologies Office
- DOE [DE-AC02-06CH11357]
- National Natural Science Fund for Innovative Research Groups [51621003]
- National Key Research and Development Program of China [2016YFB0700700]
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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 LiNi1/3Mn1/3Co1/3O2 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.
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