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Elucidating Heterogeneous Li Insertion Using Single-Crystalline and Freestanding Layered Oxide Thin Film.

Jinkyu Chung1, Chihyun Nam1, Jae Young Kim2

  • 1Department of Chemistry, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul 08826, Republic of Korea.

Nano Letters
|October 15, 2024
PubMed
Summary

Uniform lithium insertion in layered-oxide batteries is key for performance. This study reveals heterogeneous lithium concentration evolution in NMC111 due to varied insertion rates across channels, impacting battery life.

Keywords:
Lithium-ion batteryin situ imagingin situ scanning transmission X-ray microscopyinterfacial charge transferlayered oxidesingle-crystalline thin film

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Battery Technology

Background:

  • Interfacial ion insertion kinetics are critical for uniform electrochemical reactions and lithium-ion battery performance.
  • Understanding lithium insertion heterogeneity in layered-oxide battery particles is challenging due to undefined crystal orientation and diffusion lengths.

Purpose of the Study:

  • To systematically investigate lithium insertion kinetics at crystallographically defined interfaces.
  • To spatially resolve lithium insertion and map lithium concentration in situ within battery materials.

Main Methods:

  • Fabrication of a freestanding, (104)-oriented LiNi1/3Mn1/3Co1/3O2 (NMC111) single-crystal thin film using dissolution-induced release.
  • In situ scanning-transmission X-ray microscopy (STXM) for spatially resolved lithium-concentration mapping at well-defined interfaces.

Main Results:

  • Observed heterogeneous lithium-concentration evolution, indicating channel-by-channel variation in insertion rates.
  • Demonstrated that increasing current density exacerbates this heterogeneity in NMC111.
  • Identified that channel-by-channel insertion rate variation occurs despite the potential for homogeneous distribution via a solid-solution phase.

Conclusions:

  • Findings provide critical insights into battery electrode utilization and lifetime management.
  • Highlights the importance of understanding interfacial kinetics for designing efficient and durable lithium-ion batteries.
  • Suggests that controlling insertion channel activation is key for optimizing battery performance.