Multiscale Defect Regulation of Cobalt-Free Layered Oxides for High-Energy and Long-Lasting Cathodes

Reducing the reliance on cobalt in electrode chemistry is a promising step toward more sustainable and cost-effective lithium-ion batteries. However, the elimination of cobalt in layered oxides generally results in a significant decrease in capacity and/or a compromised cycle stability. Herein, we show that these intertwined issues of the cobaltless systems can be remedied by meticulously tailoring inherent defects induced at multiscale. It is demonstrated that a simple excess incorporation of lithium in the structure can effectively reduce the cation disorder and unexpectedly alter the microstructure forming routes, thereby enhancing electro-chemo-mechanical stabilities of layered cathodes. Our investigations reveal that this surplus lithium facilitates topotactic lithiation of precursors during calcination, rendering mechanically robust particles with fewer nanoporous defects and reduced cation disorder. Defect-regulated cobalt-free layered oxides successfully deliver a reversible capacity of 189 mAh g–1 at 0.5C with a retention of ∼85% after 300 cycles under commercial-level electrode loading.

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Publication Details

Journal
ACS Energy Letters
Published
2025-03-11
DOI
https://doi.org/10.1021/acsenergylett.5c00207
Citations
6
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
4.38
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article

Multiscale Defect Regulation of Cobalt-Free Layered Oxides for High-Energy and Long-Lasting Cathodes

Jaesub Kwon, Hyeokjun Park, Hyungsub Kim, Jaehoon Heo et al.
6 citations
ACS Energy Letters
Advancements in Battery Materials
4.38
article

Multiscale Defect Regulation of Cobalt-Free Layered Oxides for High-Energy and Long-Lasting Cathodes

Jaesub Kwon, Hyeokjun Park, Hyungsub Kim, Jaehoon Heo, Yun Seog Lee, Sungjae Seo, Wonju Kim, Kun‐Hee Ko, Sangwook Han, Jaesang Yoon, Kisuk Kang, Seok Hyun Song, Jongwoo Lim, Jooha Park, Sunyoung Lee, Yong‐Tae Kim, Eugene Choi
article en
6 citations

Abstract

Reducing the reliance on cobalt in electrode chemistry is a promising step toward more sustainable and cost-effective lithium-ion batteries. However, the elimination of cobalt in layered oxides generally results in a significant decrease in capacity and/or a compromised cycle stability. Herein, we show that these intertwined issues of the cobaltless systems can be remedied by meticulously tailoring inherent defects induced at multiscale. It is demonstrated that a simple excess incorporation of lithium in the structure can effectively reduce the cation disorder and unexpectedly alter the microstructure forming routes, thereby enhancing electro-chemo-mechanical stabilities of layered cathodes. Our investigations reveal that this surplus lithium facilitates topotactic lithiation of precursors during calcination, rendering mechanically robust particles with fewer nanoporous defects and reduced cation disorder. Defect-regulated cobalt-free layered oxides successfully deliver a reversible capacity of 189 mAh g–1 at 0.5C with a retention of ∼85% after 300 cycles under commercial-level electrode loading.

ACS Energy LettersVol. 10(4)
Pohang University of Science and Technology (KR), Seoul National University (KR), Korea Atomic Energy Research Institute (KR), Samsung (South Korea) (KR), Korea Research Institute of Standards and Science (KR), China Spallation Neutron Source (CN)
Affordable and clean energy
Openalex Percentile: Top 6%
Advancements in Battery Materials
4.38
DOIOpen Access PDFOpenAlex
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