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Nano Research 2023, 16(5): 6805-6814 https://doi.org/10.1007/s12274-022-5333-z
Research Article | Issue | Published: 06 February 2023

A double-layer covered architecture with spinel phase induced by LiPP for Co-free Li-rich cathode with high-rate performance and long lifespan

Show Author's Information Ruiqi Zhao1,3,  Manman Wu1,2,3,  Peixin Jiao3,4,5,  Xueting Wang1,3,  Jie Zhu1,3,  Yang Zhao1,3,  Hongtao Zhang1,3( ),  Kai Zhang3,4,5,  Chenxi Li1,3,  Yanfeng Ma1,3,  Yongsheng Chen1,2,3( )
The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin 300071, China
State Key Laboratory of Elemento-Organic Chemistry, Nankai University, Tianjin 300071, China
Renewable Energy Conversion and Storage Center (RECAST), Nankai University, Tianjin 300071, China
Department Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, China
Engineering Research Center of High-efficiency Energy Storage (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, China
Keywords:
long cycle life, Co-free Li-rich layered oxides, double-layer covered architecture, lithium polyphosphate, high-rate performance
Topics:
Energy storageLithium batteries
Cite this article:
Zhao R, Wu M, Jiao P, et al. A double-layer covered architecture with spinel phase induced by LiPP for Co-free Li-rich cathode with high-rate performance and long lifespan. Nano Research, 2023, 16(5): 6805-6814. https://doi.org/10.1007/s12274-022-5333-z
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Abstract Full text Electronic supplementary material About this article

Co-free Li-rich Mn-based layered oxides are promising candidates for next-generation lithium-ion batteries (LIBs) due to their high specific capacity, high voltage, and low cost. However, their commercialization is hindered by limited cycle life and poor rate performance. Herein, an in-situ simple and low-cost strategy with a nanoscale double-layer architecture of lithium polyphosphate (LiPP) and spinel phase covered on top of the bulk layered phase, is developed for Li1.2Mn0.6Ni0.2O2 (LMNO) using Li+-conductor LiPP (denoted as LMNO@S-LiPP). With such a double-layer covered architecture, the half-cell of LMNO@S-LiPP delivers an extremely high capacity of 202.5 mAh·g−1 at 1 A·g−1 and retains 85.3% of the initial capacity after 300 cycles, so far, the best high-rate electrochemical performance of all the previously reported LMNOs. The energy density of the full-cell assembled with commercial graphite reaches 620.9 Wh·kg−1 (based on total weight of active materials in cathode and anode). Mechanism studies indicate that the superior electrochemical performance of LMNO@S-LiPP is originated from such a nanoscale double-layer covered architecture, which accelerates Li-ion diffusion, restrains oxygen release, inhibits interfacial side reactions, and suppresses structural degradation during cycling. Moreover, this strategy is applicable for other high-energy-density cathodes, such as LiNi0.8Co0.1Mn0.1O2, Li1.2Ni0.13Co0.13Mn0.54O2, and LiCoO2. Hence, this work presents a simple, cost-effective, and scalable strategy for the development of high-performance cathode materials.


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Electronic supplementary material
About this article

A double-layer covered architecture with spinel phase induced by LiPP for Co-free Li-rich cathode with high-rate performance and long lifespan

Show Author's information Ruiqi Zhao1,3, Manman Wu1,2,3, Peixin Jiao3,4,5, Xueting Wang1,3, Jie Zhu1,3, Yang Zhao1,3, Hongtao Zhang1,3( ), Kai Zhang3,4,5, Chenxi Li1,3, Yanfeng Ma1,3, Yongsheng Chen1,2,3( )
The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin 300071, China
State Key Laboratory of Elemento-Organic Chemistry, Nankai University, Tianjin 300071, China
Renewable Energy Conversion and Storage Center (RECAST), Nankai University, Tianjin 300071, China
Department Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, China
Engineering Research Center of High-efficiency Energy Storage (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, China

Abstract

Co-free Li-rich Mn-based layered oxides are promising candidates for next-generation lithium-ion batteries (LIBs) due to their high specific capacity, high voltage, and low cost. However, their commercialization is hindered by limited cycle life and poor rate performance. Herein, an in-situ simple and low-cost strategy with a nanoscale double-layer architecture of lithium polyphosphate (LiPP) and spinel phase covered on top of the bulk layered phase, is developed for Li1.2Mn0.6Ni0.2O2 (LMNO) using Li+-conductor LiPP (denoted as LMNO@S-LiPP). With such a double-layer covered architecture, the half-cell of LMNO@S-LiPP delivers an extremely high capacity of 202.5 mAh·g−1 at 1 A·g−1 and retains 85.3% of the initial capacity after 300 cycles, so far, the best high-rate electrochemical performance of all the previously reported LMNOs. The energy density of the full-cell assembled with commercial graphite reaches 620.9 Wh·kg−1 (based on total weight of active materials in cathode and anode). Mechanism studies indicate that the superior electrochemical performance of LMNO@S-LiPP is originated from such a nanoscale double-layer covered architecture, which accelerates Li-ion diffusion, restrains oxygen release, inhibits interfacial side reactions, and suppresses structural degradation during cycling. Moreover, this strategy is applicable for other high-energy-density cathodes, such as LiNi0.8Co0.1Mn0.1O2, Li1.2Ni0.13Co0.13Mn0.54O2, and LiCoO2. Hence, this work presents a simple, cost-effective, and scalable strategy for the development of high-performance cathode materials.

Keywords: long cycle life, Co-free Li-rich layered oxides, double-layer covered architecture, lithium polyphosphate, high-rate performance

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Publication history
Copyright
Acknowledgements

Publication history

Received: 26 August 2022
Revised: 05 November 2022
Accepted: 16 November 2022
Published: 06 February 2023
Issue date: May 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

The authors gratefully acknowledge the financial support from the Ministry of Science and Technology of China (MoST, No. 52090034) and the Higher Education Discipline Innovation Project (No. B12015).

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