Lattice and Local Electronic Structure Modulation Enables Ultra-Long-Life Li-Rich Cathode Materials

Xiao Han; Renkang Wu; Guiyang Gao; Jiantao Li; Mengjian Fan; Shihao Wang; Yuanyuan Liu; Saichao Li; Liang Lin; Yinggan Zhang; Baisheng Sa; Jie Lin; Laisen Wang; Dong Liang Peng; Qingshui Xie; Khalil Amine

doi:10.1021/acsenergylett.4c00939

Lattice and Local Electronic Structure Modulation Enables Ultra-Long-Life Li-Rich Cathode Materials

Xiao Han, Renkang Wu, Guiyang Gao, Jiantao Li^*, Mengjian Fan, Shihao Wang, Yuanyuan Liu, Saichao Li, Liang Lin, Yinggan Zhang, Baisheng Sa, Jie Lin, Laisen Wang, Dong Liang Peng^*, Qingshui Xie^*, Khalil Amine^*

^*Corresponding author for this work

Chemical and Biological Engineering

Research output: Contribution to journal › Article › peer-review

8 Scopus citations

Abstract

Effectively alleviating severe performance deterioration including rapid capacity decay and continuous voltage fading of Li-rich layered oxide (LLO) cathodes by suppressing the irreversible oxygen release and transition metal (TM) migration is a critical challenge during prolonged cycling. Herein, we report a Sb-doped LLO (SLLO) cathode with shortened TM_oct-TM_oct distance and modulated local electronic structure, which can significantly enhance the oxygen vacancy formation energy and TM migration energy barriers. Therefore, the SLLO cathode showcases an impressive energy density of 1052 Wh kg^-1 at 0.2 C and an outstanding rate capability of 214 mAh g^-1 at 5 C with a remarkable capacity retention of 79.2% even after 1000 cycles. It should be pointed out that it exhibits greatly enhanced voltage stability with an outstanding voltage retention of 86.2% after cycling 1600 times at 10 C. This work provides a prototype for significantly enhancing the reversibility in electrochemical reactions of high-capacity layered cathode materials.

Original language	English (US)
Pages (from-to)	3219-3226
Number of pages	8
Journal	ACS Energy Letters
Volume	9
Issue number	7
DOIs	https://doi.org/10.1021/acsenergylett.4c00939
State	Published - Jul 12 2024

Funding

The authors gratefully acknowledge financial support from the National Natural Science Foundation of China (Grant Nos. 51931006, 52272240, and U22A20118), Science and Technology Planning Projects of Fujian Province of China (Grant No. 2023H0003), the Fundamental Research Funds for the Central Universities of China (Xiamen University: No. 20720220074), and the \u201CDouble-First Class\u201D Foundation of Materials Intelligent Manufacturing Discipline of Xiamen University. This work gratefully acknowledges support from the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office.

ASJC Scopus subject areas

Chemistry (miscellaneous)
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology
Materials Chemistry

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title = "Lattice and Local Electronic Structure Modulation Enables Ultra-Long-Life Li-Rich Cathode Materials",

abstract = "Effectively alleviating severe performance deterioration including rapid capacity decay and continuous voltage fading of Li-rich layered oxide (LLO) cathodes by suppressing the irreversible oxygen release and transition metal (TM) migration is a critical challenge during prolonged cycling. Herein, we report a Sb-doped LLO (SLLO) cathode with shortened TMoct-TMoct distance and modulated local electronic structure, which can significantly enhance the oxygen vacancy formation energy and TM migration energy barriers. Therefore, the SLLO cathode showcases an impressive energy density of 1052 Wh kg-1 at 0.2 C and an outstanding rate capability of 214 mAh g-1 at 5 C with a remarkable capacity retention of 79.2% even after 1000 cycles. It should be pointed out that it exhibits greatly enhanced voltage stability with an outstanding voltage retention of 86.2% after cycling 1600 times at 10 C. This work provides a prototype for significantly enhancing the reversibility in electrochemical reactions of high-capacity layered cathode materials.",

author = "Xiao Han and Renkang Wu and Guiyang Gao and Jiantao Li and Mengjian Fan and Shihao Wang and Yuanyuan Liu and Saichao Li and Liang Lin and Yinggan Zhang and Baisheng Sa and Jie Lin and Laisen Wang and Peng, {Dong Liang} and Qingshui Xie and Khalil Amine",

note = "Publisher Copyright: {\textcopyright} 2024 UChicago Argonne, LLC, Operator of Argonne National Laboratory. Published by American Chemical Society.",

year = "2024",

month = jul,

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doi = "10.1021/acsenergylett.4c00939",

language = "English (US)",

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T1 - Lattice and Local Electronic Structure Modulation Enables Ultra-Long-Life Li-Rich Cathode Materials

AU - Han, Xiao

AU - Wu, Renkang

AU - Gao, Guiyang

AU - Li, Jiantao

AU - Fan, Mengjian

AU - Wang, Shihao

AU - Liu, Yuanyuan

AU - Li, Saichao

AU - Lin, Liang

AU - Zhang, Yinggan

AU - Sa, Baisheng

AU - Lin, Jie

AU - Wang, Laisen

AU - Peng, Dong Liang

AU - Xie, Qingshui

AU - Amine, Khalil

PY - 2024/7/12

Y1 - 2024/7/12

N2 - Effectively alleviating severe performance deterioration including rapid capacity decay and continuous voltage fading of Li-rich layered oxide (LLO) cathodes by suppressing the irreversible oxygen release and transition metal (TM) migration is a critical challenge during prolonged cycling. Herein, we report a Sb-doped LLO (SLLO) cathode with shortened TMoct-TMoct distance and modulated local electronic structure, which can significantly enhance the oxygen vacancy formation energy and TM migration energy barriers. Therefore, the SLLO cathode showcases an impressive energy density of 1052 Wh kg-1 at 0.2 C and an outstanding rate capability of 214 mAh g-1 at 5 C with a remarkable capacity retention of 79.2% even after 1000 cycles. It should be pointed out that it exhibits greatly enhanced voltage stability with an outstanding voltage retention of 86.2% after cycling 1600 times at 10 C. This work provides a prototype for significantly enhancing the reversibility in electrochemical reactions of high-capacity layered cathode materials.

AB - Effectively alleviating severe performance deterioration including rapid capacity decay and continuous voltage fading of Li-rich layered oxide (LLO) cathodes by suppressing the irreversible oxygen release and transition metal (TM) migration is a critical challenge during prolonged cycling. Herein, we report a Sb-doped LLO (SLLO) cathode with shortened TMoct-TMoct distance and modulated local electronic structure, which can significantly enhance the oxygen vacancy formation energy and TM migration energy barriers. Therefore, the SLLO cathode showcases an impressive energy density of 1052 Wh kg-1 at 0.2 C and an outstanding rate capability of 214 mAh g-1 at 5 C with a remarkable capacity retention of 79.2% even after 1000 cycles. It should be pointed out that it exhibits greatly enhanced voltage stability with an outstanding voltage retention of 86.2% after cycling 1600 times at 10 C. This work provides a prototype for significantly enhancing the reversibility in electrochemical reactions of high-capacity layered cathode materials.

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Lattice and Local Electronic Structure Modulation Enables Ultra-Long-Life Li-Rich Cathode Materials

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