ACS_Nano Letters
November 20, 2024
Volume 24, Issue 46
Pages 14541-14908
Elucidating Heterogeneous Li Insertion Using Single-Crystalline and Freestanding Layered Oxide Thin Film
The kinetics of interfacial ion insertion govern the uniformity of electrochemical reactions, playing a crucial role in lithium-ion battery performance. In two-dimensional lithium-conducting layered-oxide battery particles, variation in insertion rates across insertion channels remains unclear due to poorly defined crystal orientation at the solid–liquid interface and solid-state-lithium-diffusion length. This ambiguity complicates understanding inhomogeneous lithium-insertion channels activation. A systematic study requires crystallographically predefined interfaces and in situ lithium-concentration mapping. Here, we fabricated a freestanding, (104)-oriented-LiNi1/3Mn1/3Co1/3O2 single-crystal thin film using dissolution-induced release and performed in situ scanning-transmission-X-ray-microscopy to spatially resolve lithium-insertion at well-defined-interfaces. We observed heterogeneous lithium-concentration evolution due to channel-by-channel insertion rate variation, despite the potential for homogeneous lithium distribution via a solid-solution-phase at equilibrium in NMC111. Increasing current density exacerbates this heterogeneity, highlighting channel-by-channel variation. Our findings provide critical insights into battery electrode utilization and lifetime management, potentially guiding the design of more efficient and durable lithium-ion batteries.
- Jinkyu Chung
- Chihyun Nam
- Jae Young Kim
- Tae Hyung Lee
- Juwon Kim
- Danwon Lee
- Bonho Koo
- Sugeun Jo
- Jeongho Cho
- Sebastian Kunze
- Yong Seok Choi
- Jaejung Song
- Hanbi Choi
- Jiseok Kim
- Sung Hyuk Park
- Hyeonji Lee
- Byung Hee Hong
- Namdong Kim
- David A. Shapiro
- Ho Won Jang
- Jongwoo Lim
https://pubs.acs.org/doi/10.1021/acs.nanolett.4c04129
Image created by minjeong Kim / Nanosphere
ACS_Nano Letters
November 20, 2024
Volume 24, Issue 46
Pages 14541-14908
Elucidating Heterogeneous Li Insertion Using Single-Crystalline and Freestanding Layered Oxide Thin Film
The kinetics of interfacial ion insertion govern the uniformity of electrochemical reactions, playing a crucial role in lithium-ion battery performance. In two-dimensional lithium-conducting layered-oxide battery particles, variation in insertion rates across insertion channels remains unclear due to poorly defined crystal orientation at the solid–liquid interface and solid-state-lithium-diffusion length. This ambiguity complicates understanding inhomogeneous lithium-insertion channels activation. A systematic study requires crystallographically predefined interfaces and in situ lithium-concentration mapping. Here, we fabricated a freestanding, (104)-oriented-LiNi1/3Mn1/3Co1/3O2 single-crystal thin film using dissolution-induced release and performed in situ scanning-transmission-X-ray-microscopy to spatially resolve lithium-insertion at well-defined-interfaces. We observed heterogeneous lithium-concentration evolution due to channel-by-channel insertion rate variation, despite the potential for homogeneous lithium distribution via a solid-solution-phase at equilibrium in NMC111. Increasing current density exacerbates this heterogeneity, highlighting channel-by-channel variation. Our findings provide critical insights into battery electrode utilization and lifetime management, potentially guiding the design of more efficient and durable lithium-ion batteries.
https://pubs.acs.org/doi/10.1021/acs.nanolett.4c04129
Image created by minjeong Kim / Nanosphere