Microstructural Evolution Dynamics in Rapid Joule Heating Densification of High‐Nickel Cathodes

High-energy density materials are essential for the advancement of next-generation lithium-ion batteries, which power a wide range of applications from portable electronics to electric vehicles. Among them, high-Nickel (Ni) layered oxide cathodes have emerged as promising candidates due to their high capacity and cost-effectiveness. However, pores and excessive grain growth in high-Ni layered oxides compromise energy density and mechanical integrity, while oversized grains hinder lithium-ion diffusion kinetics, necessitating a sintering strategy that promotes densification without inducing abnormal grain growth. Here, a rapid Joule heating technique combined with two-step sintering is introduced that significantly improves the microstructural integrity of high-Ni cathodes. This approach enables fast densification while suppressing grain growth, resulting in cathodes with higher density, reduced porosity, and enhanced mechanical strength. Through in situ X-ray diffraction (XRD), small angle X-ray scattering (SAXS), and 3D ptychography analysis, it is found that the rapid Joule-heated cathodes exhibit mitigated phase separation, suppressed pore evolution, and improved resistance to crack propagation. They deliver superior cycling stability, coulombic efficiency, and rate performance. These results provide insights into the relationship between sintering dynamics and microstructural evolution, offering guidelines for synthesizing fully densified, high-energy density materials.

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Publication Details

Journal
Advanced Materials
Published
2025-08-04
DOI
https://doi.org/10.1002/adma.202508602
Citations
9
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
6.57

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Microstructural Evolution Dynamics in Rapid Joule Heating Densification of High‐Nickel Cathodes

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Advancements in Battery Materials
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Microstructural Evolution Dynamics in Rapid Joule Heating Densification of High‐Nickel Cathodes

Euna Kim, Yuzhang Li, Won Kyung Seong, Jaeyong Shin, Sang‐Chae Jeon, Su Yong Lee, Hyun‐Wook Lee, Wooyoung Jin, Myeongjun Choi, Sunghwan Jin, Rodney S. Ruoff, Changyong Song, Min‐Ho Kim, Eunyoung Park, Ji‐Seon Seo, Ahreum Choi
article en
9 citations

Abstract

High-energy density materials are essential for the advancement of next-generation lithium-ion batteries, which power a wide range of applications from portable electronics to electric vehicles. Among them, high-Nickel (Ni) layered oxide cathodes have emerged as promising candidates due to their high capacity and cost-effectiveness. However, pores and excessive grain growth in high-Ni layered oxides compromise energy density and mechanical integrity, while oversized grains hinder lithium-ion diffusion kinetics, necessitating a sintering strategy that promotes densification without inducing abnormal grain growth. Here, a rapid Joule heating technique combined with two-step sintering is introduced that significantly improves the microstructural integrity of high-Ni cathodes. This approach enables fast densification while suppressing grain growth, resulting in cathodes with higher density, reduced porosity, and enhanced mechanical strength. Through in situ X-ray diffraction (XRD), small angle X-ray scattering (SAXS), and 3D ptychography analysis, it is found that the rapid Joule-heated cathodes exhibit mitigated phase separation, suppressed pore evolution, and improved resistance to crack propagation. They deliver superior cycling stability, coulombic efficiency, and rate performance. These results provide insights into the relationship between sintering dynamics and microstructural evolution, offering guidelines for synthesizing fully densified, high-energy density materials.

Advanced MaterialsVol. 37(45)
Pohang University of Science and Technology (KR), University of California, Los Angeles (US), Kangwon National University (KR), Changwon National University (KR), Advanced Energy (United States) (US), Institute for Basic Science (KR), Ulsan National Institute of Science and Technology (KR)
National Research Foundation, Pohang University of Science and Technology, Ulsan National Institute of Science and Technology, Ministry of Education, National Research Foundation of Korea, Ministry of Education, India, Institute for Basic Science, Ministry of Science and ICT, South Korea
Affordable and clean energy
Openalex Percentile: Top 3%
Advancements in Battery Materials
6.57
DOIOpen Access PDFOpenAlex
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