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Achievement of lithium (Li) metal anode with thin thickness (e.g., ≤ 30 µm) is highly desirable for rechargeable high energy density batteries. However, the fabrication and application of such thin Li metal foil electrode remain challenging due to the poor mechanical processibility and inferior electrochemical performance of metallic Li. Here, mechanico-chemical synthesis of robust ultrathin Li/Li3P (LLP) composite foils (~ 15 µm) is demonstrated by employing repeated mechanical rolling/stacking operations using red P and metallic Li as raw materials. The in-situ formed Li+-conductive Li3P nanoparticles in metallic Li matrix and their tight bonding strengthen the mechanical durability and enable the successful fabrication of free-standing ultrathin Li metal composite foil. Besides, it also reduces the electrochemical Li nucleation barrier and homogenizes Li plating/stripping behavior. When matching to high-voltage LiCoO2, the full cell with a low negative/positive (N/P) capacity ratio of ~ 1.5 offers a high energy density of ~ 522 W·h·kg−1 at 0.5 C based on the mass of cathode and anode. Taking into account its facile manufacturing, potentially low cost, and good electrochemical performance, we believe that such an ultrathin composite Li metal foil design with nanoparticle-dispersion-strengthened mechanism may boost the development of high energy density Li metal batteries.


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A Li3P nanoparticle dispersion strengthened ultrathin Li metal electrode for high energy density rechargeable batteries

Show Author's information Lin Fu1,2,§Xiancheng Wang2,§Bao Zhang3Zihe Chen2Yuanjian Li2,4Yongming Sun2( )
Provincial Guizhou Key Laboratory of Green Chemical and Clean Energy Technology, School of Chemistry and Chemical Engineering, Guizhou University, Guiyang 550025, China
Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan 430074, China
School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore 637371, Singapore
Institute of Materials Research and Engineering, Agency for Science Technology and Research (A*STAR), Singapore 138634, Singapore

§ Lin Fu and Xiancheng Wang contributed equally to this work.

Abstract

Achievement of lithium (Li) metal anode with thin thickness (e.g., ≤ 30 µm) is highly desirable for rechargeable high energy density batteries. However, the fabrication and application of such thin Li metal foil electrode remain challenging due to the poor mechanical processibility and inferior electrochemical performance of metallic Li. Here, mechanico-chemical synthesis of robust ultrathin Li/Li3P (LLP) composite foils (~ 15 µm) is demonstrated by employing repeated mechanical rolling/stacking operations using red P and metallic Li as raw materials. The in-situ formed Li+-conductive Li3P nanoparticles in metallic Li matrix and their tight bonding strengthen the mechanical durability and enable the successful fabrication of free-standing ultrathin Li metal composite foil. Besides, it also reduces the electrochemical Li nucleation barrier and homogenizes Li plating/stripping behavior. When matching to high-voltage LiCoO2, the full cell with a low negative/positive (N/P) capacity ratio of ~ 1.5 offers a high energy density of ~ 522 W·h·kg−1 at 0.5 C based on the mass of cathode and anode. Taking into account its facile manufacturing, potentially low cost, and good electrochemical performance, we believe that such an ultrathin composite Li metal foil design with nanoparticle-dispersion-strengthened mechanism may boost the development of high energy density Li metal batteries.

Keywords: lithium metal anode, high energy density battery, mechanico-chemical synthesis, ultrathin Li/Li3P composite foil, low negative/positive capacity ratio

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Publication history
Copyright
Acknowledgements

Publication history

Received: 09 August 2023
Revised: 07 October 2023
Accepted: 18 October 2023
Published: 02 January 2024
Issue date: May 2024

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

Y. S. acknowledges the financial support by National Natural Science Foundation of China (No. 52272207). L. F. thanks the financial support by National Natural Science Foundation of China (No. 22209031), Guizhou Provincial Basic Research Program (Natural Science) (No. QKHJC-ZK[2023]YB046), and Natural Science Special Foundation of Guizhou University (No. X2022122 Special Post B).

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