Strain-associated nanoscale fluctuating lithium transport within single-crystalline LiNi1/3Mn1/3Co1/3O2 cathode particles

Danwon Lee, Chihyun Nam, Juwon Kim, Sooseong Hwang, Bonho Koo, Hyejeong Hyun, Jinkyu Chung, Sungjae Seo, Munsoo Song, Jaejung Song, Myeongjun Kim, Daan Hein Alsem, Norman J. Salmon, Suyong Lee, Yeonchoo Cho, Namdong Kim, David A. Shapiro and Jongwoo Lim ()
Additional contact information
Danwon Lee: Seoul National University
Chihyun Nam: Seoul National University
Juwon Kim: Seoul National University
Sooseong Hwang: Seoul National University
Bonho Koo: Seoul National University
Hyejeong Hyun: Seoul National University
Jinkyu Chung: Seoul National University
Sungjae Seo: Seoul National University
Munsoo Song: Seoul National University
Jaejung Song: Seoul National University
Myeongjun Kim: Seoul National University
Daan Hein Alsem: Hummingbird Scientific
Norman J. Salmon: Hummingbird Scientific
Suyong Lee: Pohang University of Science and Technology
Yeonchoo Cho: Samsung Electronics
Namdong Kim: Pohang University of Science and Technology
David A. Shapiro: Lawrence Berkeley National Laboratory
Jongwoo Lim: Seoul National University

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Solid-state lithium diffusion dynamics are critical for the rate capability and longevity of Li-ion batteries. Conventionally, nanoscale lithium diffusion within individual battery particles has been simplified as being primarily driven by concentration gradients, despite the associated processes inducing local lattice expansion, contraction, and strain fields. Using operando scanning transmission soft X-ray microscopy with high spatial resolution and chemical sensitivity to track nanoscale intraparticle lithium transport, and post-cycling Bragg coherent diffraction X-ray imaging to directly reveal three-dimensional intraparticle strain fields, we uncover strain-associated lithium transport dynamics within single-crystalline LiNi1/3Mn1/3Co1/3O2 (scNMC) particles during cycling. Contrary to the expected thermodynamic solid-solution behavior of scNMC, our observations reveal near-uniform but fluctuating regions of lithium-dense and lithium-dilute areas during cycling. These fluctuations suggest that nanoscale lithium diffusion can proceed counter to concentration gradients. Additionally, we demonstrate that an increased presence of lithium-dilute regions near the surface enhances lithium surface insertion kinetics, emphasizing the importance of controlling surface lithium distribution to improve rate performance. Our study provides insights into nanoscale solid-state ion transport, with potential applications in batteries, solid-state fuel cells, and memristors.

Date: 2025
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DOI: 10.1038/s41467-025-64068-9

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