Co-free gradient lithium-rich cathode for high-energy batteries with optimized cyclability - Details

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Abstract：

Lithium-rich　layered　oxides　(LLOs)　hold　the　promise　for　high-energy　battery　cathodes.　However,　its　application　has　been　hindered　by　voltage　decay　associated　with　irreversible　reactions　at　high　voltages　despite　decades　of　intensive　efforts.　Here,　we　first　theoretically　studied　the　molecular　orbitals　of　Mn-based　Li-rich　configurations.　We　found　that　the　π-bond　ring　formed　within　the　LiMn6　structure　could　participate　in　stable　redox　reactions　as　one　unit,　but　Co　could　disrupt　its　symmetry.　We　thus　designed　and　synthesized　Co-free　concentration-gradient　LLOs　(CF-CG-LLOs)　materials.　The　combination　of　concentration　gradient　and　Co　removal　leads　to　exceptional　capacity　retention　without　any　fading　over　100　cycles　of　the　pouch　cell.　More　importantly,　it　exhibits　an　extraordinarily　low　voltage　decay　of　0.15　mV/cycle,　accompanied　by　a　high　Coulombic　efficiency　of　99.86%.　This　concept　and　demonstration　of　CF-CG-LLO　cathodes　reveal　a　viable　avenue　toward　low-cost,　high-energy-density　battery　cathodes.　Copyright　©　2024　the　Author(s).　Published　by　PNAS.

Keyword：

redox mechanism lithium ion batteries concentration gradient battery cathode lithium-rich layered oxides

Author Community：

[ 1 ] [Yang H.]Institute of Advanced Battery Materials and Devices, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 2 ] [Yang H.]Key Laboratory of Advanced Functional Materials, Ministry of Education, Beijing University of Technology, Beijing, 100124, China
[ 3 ] [Wang L.]Institute of Advanced Battery Materials and Devices, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 4 ] [Wang L.]Key Laboratory of Advanced Functional Materials, Ministry of Education, Beijing University of Technology, Beijing, 100124, China
[ 5 ] [Li Y.]Institute of Advanced Battery Materials and Devices, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 6 ] [Li Y.]Key Laboratory of Advanced Functional Materials, Ministry of Education, Beijing University of Technology, Beijing, 100124, China
[ 7 ] [Zhuo Z.]The Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, 94720, CA, United States
[ 8 ] [Wu T.]Institute of Advanced Battery Materials and Devices, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 9 ] [Wu T.]Key Laboratory of Advanced Functional Materials, Ministry of Education, Beijing University of Technology, Beijing, 100124, China
[ 10 ] [Liu J.]Center for High Pressure Science and Technology Advanced Research, Beijing, 100193, China
[ 11 ] [Liu J.]College of Materials Science and Engineering, University of Science and Technology Beijing, Beijing, 100083, China
[ 12 ] [Xu L.]Center for High Pressure Science and Technology Advanced Research, Beijing, 100193, China
[ 13 ] [Xu L.]College of Materials Science and Engineering, University of Science and Technology Beijing, Beijing, 100083, China
[ 14 ] [Du H.]Institute of Advanced Battery Materials and Devices, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 15 ] [Du H.]Key Laboratory of Advanced Functional Materials, Ministry of Education, Beijing University of Technology, Beijing, 100124, China
[ 16 ] [Liu S.]Institute of Advanced Battery Materials and Devices, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 17 ] [Liu S.]Key Laboratory of Advanced Functional Materials, Ministry of Education, Beijing University of Technology, Beijing, 100124, China
[ 18 ] [Wu L.]Institute of Advanced Battery Materials and Devices, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 19 ] [Wu L.]Key Laboratory of Advanced Functional Materials, Ministry of Education, Beijing University of Technology, Beijing, 100124, China
[ 20 ] [Zhao S.]Institute of Advanced Battery Materials and Devices, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 21 ] [Zhao S.]Key Laboratory of Advanced Functional Materials, Ministry of Education, Beijing University of Technology, Beijing, 100124, China
[ 22 ] [Tang M.]Center for High Pressure Science and Technology Advanced Research, Beijing, 100193, China
[ 23 ] [Tang M.]College of Materials Science and Engineering, University of Science and Technology Beijing, Beijing, 100083, China
[ 24 ] [Yang W.]The Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, 94720, CA, United States
[ 25 ] [Yu H.]Institute of Advanced Battery Materials and Devices, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 26 ] [Yu H.]Key Laboratory of Advanced Functional Materials, Ministry of Education, Beijing University of Technology, Beijing, 100124, China

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Related Keywords：

Full Concentration Gradient-Tailored Li-Rich Layered Oxides for High-Energy Lithium-Ion Batteries.
2021，Advanced materials
Gradient "Single-Crystal" Li-Rich Cathode Materials for High-Stable Lithium-Ion Batteries
2022，ADVANCED FUNCTIONAL MATERIALS
Thermal Stability Enhancement through Structure Modification on the Microsized Crystalline Grain Surface of Lithium-Rich Layered Oxides
2020，ACS APPLIED MATERIALS & INTERFACES
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Source ：

Proceedings of the National Academy of Sciences of the United States of America

ISSN： 0027-8424

Year： 2024

Issue： 50

Volume： 121

1 1 . 1 0 0

JCR@2022

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WoS CC Cited Count：

SCOPUS Cited Count： 5

ESI Highly Cited Papers on the List： 0 Unfold All

WanFang Cited Count：

Chinese Cited Count：

30 Days PV： 9

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