Li-rich oxide micro-bricks with exposed {010} planes to construct ultrahigh-compaction hierarchical cathodes for Li-ion batteries

Although lithium-rich manganese-based (LRM) cathode materials have high capacity (> ​250 ​mAh ​g−1) due to their multi-electron redox mechanisms and offer cost advantages due to their high Mn content, challenges remain before they can achieve commercialization as replacements for lithium cobalt o...

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Main Authors: Yongjian Li, Tong Sun, Chenxing Yang, Yuefeng Su, Cai Liu, Xinyu Zhu, Yihong Wang, Siyuan Ma, Xinyu Wang, Yizhi Zhai, Wenlong Kang, Lai Chen, Meng Wang, Liang Zhang, Bin Wang, Qing Huang, Yibiao Guan, Feng Wu, Ning Li
Format: Article
Language:English
Published: KeAi Communications Co. Ltd. 2025-09-01
Series:eScience
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Online Access:http://www.sciencedirect.com/science/article/pii/S2667141725000357
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author Yongjian Li
Tong Sun
Chenxing Yang
Yuefeng Su
Cai Liu
Xinyu Zhu
Yihong Wang
Siyuan Ma
Xinyu Wang
Yizhi Zhai
Wenlong Kang
Lai Chen
Meng Wang
Liang Zhang
Bin Wang
Qing Huang
Yibiao Guan
Feng Wu
Ning Li
author_facet Yongjian Li
Tong Sun
Chenxing Yang
Yuefeng Su
Cai Liu
Xinyu Zhu
Yihong Wang
Siyuan Ma
Xinyu Wang
Yizhi Zhai
Wenlong Kang
Lai Chen
Meng Wang
Liang Zhang
Bin Wang
Qing Huang
Yibiao Guan
Feng Wu
Ning Li
author_sort Yongjian Li
collection DOAJ
description Although lithium-rich manganese-based (LRM) cathode materials have high capacity (> ​250 ​mAh ​g−1) due to their multi-electron redox mechanisms and offer cost advantages due to their high Mn content, challenges remain before they can achieve commercialization as replacements for lithium cobalt oxides which have high volumetric energy density. Here, we construct a hierarchically structured LRM cathode, featuring primary micro-bricks and abundant exposure of lithium-ion active transport facets ({010} planes). Benefiting from these densely packed bricks and rapid lithium-ion active planes, the hierarchical material achieves an optimal compaction density of 3.4 ​g ​cm−3 and an ultrahigh volumetric energy density of 3431.0 ​Wh ​L−1, which is the highest performance level to date. Advanced characterizations, including hard X-ray absorption spectra and wide-angle X-ray scattering spectra, combined with density functional theory calculations, demonstrate that the hierarchical material shows a highly reversible charge compensation process and low-strain structural evolution. In addition, when the material has appropriate Li/Ni intermixing, it is not prone to shearing or sliding along the two-dimensional lithium-ion diffusion planes, which promotes robust architectural stability under high-pressure calendering and long-term cycling. This work should promote the development of advanced cathode materials for rechargeable batteries with high volumetric energy density.
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spelling doaj-art-d006dbd8eaea47d79c19d2bd242a01c82025-08-24T05:14:55ZengKeAi Communications Co. Ltd.eScience2667-14172025-09-015510040510.1016/j.esci.2025.100405Li-rich oxide micro-bricks with exposed {010} planes to construct ultrahigh-compaction hierarchical cathodes for Li-ion batteriesYongjian Li0Tong Sun1Chenxing Yang2Yuefeng Su3Cai Liu4Xinyu Zhu5Yihong Wang6Siyuan Ma7Xinyu Wang8Yizhi Zhai9Wenlong Kang10Lai Chen11Meng Wang12Liang Zhang13Bin Wang14Qing Huang15Yibiao Guan16Feng Wu17Ning Li18School of Materials Science and Engineering, Beijing Key Laboratory of Environmental Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Chongqing Innovation Center, Beijing Institute of Technology, Chongqing 401120, ChinaSchool of Materials Science and Engineering, Beijing Key Laboratory of Environmental Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Chongqing Innovation Center, Beijing Institute of Technology, Chongqing 401120, ChinaSchool of Materials Science and Engineering, Beijing Key Laboratory of Environmental Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Chongqing Innovation Center, Beijing Institute of Technology, Chongqing 401120, ChinaSchool of Materials Science and Engineering, Beijing Key Laboratory of Environmental Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Chongqing Innovation Center, Beijing Institute of Technology, Chongqing 401120, China; Beijing Institute of Technology Zhuhai Campus, Zhuhai 519085, China; Corresponding authors.School of Materials Science and Engineering, Beijing Key Laboratory of Environmental Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Chongqing Innovation Center, Beijing Institute of Technology, Chongqing 401120, ChinaSchool of Materials Science and Engineering, Beijing Key Laboratory of Environmental Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Chongqing Innovation Center, Beijing Institute of Technology, Chongqing 401120, ChinaSchool of Materials Science and Engineering, Beijing Key Laboratory of Environmental Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Chongqing Innovation Center, Beijing Institute of Technology, Chongqing 401120, ChinaSchool of Materials Science and Engineering, Beijing Key Laboratory of Environmental Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Chongqing Innovation Center, Beijing Institute of Technology, Chongqing 401120, ChinaSchool of Materials Science and Engineering, Beijing Key Laboratory of Environmental Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Chongqing Innovation Center, Beijing Institute of Technology, Chongqing 401120, ChinaSchool of Materials Science and Engineering, Beijing Key Laboratory of Environmental Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Chongqing Innovation Center, Beijing Institute of Technology, Chongqing 401120, ChinaSchool of Materials Science and Engineering, Beijing Key Laboratory of Environmental Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Chongqing Innovation Center, Beijing Institute of Technology, Chongqing 401120, ChinaSchool of Materials Science and Engineering, Beijing Key Laboratory of Environmental Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Chongqing Innovation Center, Beijing Institute of Technology, Chongqing 401120, ChinaChongqing Innovation Center, Beijing Institute of Technology, Chongqing 401120, ChinaInstitute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou 215123, ChinaMinmetals Exploration & Development CO. LTD, Beijing 100010, ChinaSchool of Materials Science and Engineering, Beijing Key Laboratory of Environmental Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Chongqing Innovation Center, Beijing Institute of Technology, Chongqing 401120, China; Corresponding authors.China Electric Power Research Institute, Beijing 100192, China; Corresponding authors.School of Materials Science and Engineering, Beijing Key Laboratory of Environmental Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Chongqing Innovation Center, Beijing Institute of Technology, Chongqing 401120, ChinaSchool of Materials Science and Engineering, Beijing Key Laboratory of Environmental Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Chongqing Innovation Center, Beijing Institute of Technology, Chongqing 401120, China; Beijing Institute of Technology Zhuhai Campus, Zhuhai 519085, China; Corresponding authors.Although lithium-rich manganese-based (LRM) cathode materials have high capacity (> ​250 ​mAh ​g−1) due to their multi-electron redox mechanisms and offer cost advantages due to their high Mn content, challenges remain before they can achieve commercialization as replacements for lithium cobalt oxides which have high volumetric energy density. Here, we construct a hierarchically structured LRM cathode, featuring primary micro-bricks and abundant exposure of lithium-ion active transport facets ({010} planes). Benefiting from these densely packed bricks and rapid lithium-ion active planes, the hierarchical material achieves an optimal compaction density of 3.4 ​g ​cm−3 and an ultrahigh volumetric energy density of 3431.0 ​Wh ​L−1, which is the highest performance level to date. Advanced characterizations, including hard X-ray absorption spectra and wide-angle X-ray scattering spectra, combined with density functional theory calculations, demonstrate that the hierarchical material shows a highly reversible charge compensation process and low-strain structural evolution. In addition, when the material has appropriate Li/Ni intermixing, it is not prone to shearing or sliding along the two-dimensional lithium-ion diffusion planes, which promotes robust architectural stability under high-pressure calendering and long-term cycling. This work should promote the development of advanced cathode materials for rechargeable batteries with high volumetric energy density.http://www.sciencedirect.com/science/article/pii/S2667141725000357Li-rich manganese-based cathodeMicro-bricksHigh compaction densityHigh volumetric energy densityLi/Ni mixing
spellingShingle Yongjian Li
Tong Sun
Chenxing Yang
Yuefeng Su
Cai Liu
Xinyu Zhu
Yihong Wang
Siyuan Ma
Xinyu Wang
Yizhi Zhai
Wenlong Kang
Lai Chen
Meng Wang
Liang Zhang
Bin Wang
Qing Huang
Yibiao Guan
Feng Wu
Ning Li
Li-rich oxide micro-bricks with exposed {010} planes to construct ultrahigh-compaction hierarchical cathodes for Li-ion batteries
eScience
Li-rich manganese-based cathode
Micro-bricks
High compaction density
High volumetric energy density
Li/Ni mixing
title Li-rich oxide micro-bricks with exposed {010} planes to construct ultrahigh-compaction hierarchical cathodes for Li-ion batteries
title_full Li-rich oxide micro-bricks with exposed {010} planes to construct ultrahigh-compaction hierarchical cathodes for Li-ion batteries
title_fullStr Li-rich oxide micro-bricks with exposed {010} planes to construct ultrahigh-compaction hierarchical cathodes for Li-ion batteries
title_full_unstemmed Li-rich oxide micro-bricks with exposed {010} planes to construct ultrahigh-compaction hierarchical cathodes for Li-ion batteries
title_short Li-rich oxide micro-bricks with exposed {010} planes to construct ultrahigh-compaction hierarchical cathodes for Li-ion batteries
title_sort li rich oxide micro bricks with exposed 010 planes to construct ultrahigh compaction hierarchical cathodes for li ion batteries
topic Li-rich manganese-based cathode
Micro-bricks
High compaction density
High volumetric energy density
Li/Ni mixing
url http://www.sciencedirect.com/science/article/pii/S2667141725000357
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