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Lithium (Li) metal is regarded as the best anode material for lithium metal batteries (LMBs) due to its high theoretical specific capacity and low redox potential. However, the notorious dendrites growth and extreme instability of the solid electrolyte interphase (SEI) layers have severely retarded the commercialization process of LMBs. Herein, a double-layered polymer/alloy composite artificial SEI composed of a robust poly(1,3-dioxolane) (PDOL) protective layer, Sn and LiCl nanoparticles, denoted as PDOL@Sn-LiCl, is fabricated by the combination of in-situ substitution and polymerization processes on the surface of Li metal anode. The lithiophilic Sn-LiCl multiphase can supply plenty of Li-ion transport channels, contributing to the homogeneous nucleation and dense accumulation of Li metal. The mechanically tough PDOL layer can maintain the stability and compact structure of the inorganic layer in the long-term cycling, and suppress the volume fluctuation and dendrites formation of the Li metal anode. As a result, the symmetrical cell under the double-layered artificial SEI protection shows excellent cycling stability of 300 h at 5.0 mA·cm−2 for 1 mAh·cm−2. Notably, the Li||LiFePO4 full cell also exhibits enhanced capacity retention of 150.1 mAh·g−1 after 600 cycles at 1.0 C. Additionally, the protected Li foil can effectively resist the air and water corrosion, signifying the safe operation of Li metal in practical applications. This present finding proposed a different tactic to achieve safe and dendrite-free Li metal anodes with excellent cycling stability.


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In-situ constructed polymer/alloy composite with high ionic conductivity as an artificial solid electrolyte interphase to stabilize lithium metal anode

Show Author's information Ai-Long Chen1,§Yushan Qian1,§Shujun Zheng1Yuyang Chen1Yue Ouyang1Lulu Mo1Zheng-Long Xu2Yue-E Miao1( )Tianxi Liu1,3
State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China
Department of Industrial and Systems Engineering, The Hong Kong Polytechnic University, Hong Hum, Kowloon, Hong Kong 999077, China
Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, China

§ Ai-Long Chen and Yushan Qian contributed equally to this work.

Abstract

Lithium (Li) metal is regarded as the best anode material for lithium metal batteries (LMBs) due to its high theoretical specific capacity and low redox potential. However, the notorious dendrites growth and extreme instability of the solid electrolyte interphase (SEI) layers have severely retarded the commercialization process of LMBs. Herein, a double-layered polymer/alloy composite artificial SEI composed of a robust poly(1,3-dioxolane) (PDOL) protective layer, Sn and LiCl nanoparticles, denoted as PDOL@Sn-LiCl, is fabricated by the combination of in-situ substitution and polymerization processes on the surface of Li metal anode. The lithiophilic Sn-LiCl multiphase can supply plenty of Li-ion transport channels, contributing to the homogeneous nucleation and dense accumulation of Li metal. The mechanically tough PDOL layer can maintain the stability and compact structure of the inorganic layer in the long-term cycling, and suppress the volume fluctuation and dendrites formation of the Li metal anode. As a result, the symmetrical cell under the double-layered artificial SEI protection shows excellent cycling stability of 300 h at 5.0 mA·cm−2 for 1 mAh·cm−2. Notably, the Li||LiFePO4 full cell also exhibits enhanced capacity retention of 150.1 mAh·g−1 after 600 cycles at 1.0 C. Additionally, the protected Li foil can effectively resist the air and water corrosion, signifying the safe operation of Li metal in practical applications. This present finding proposed a different tactic to achieve safe and dendrite-free Li metal anodes with excellent cycling stability.

Keywords: in-situ polymerization, polymer/alloy composite, double-layered structure, artificial solid electrolyte interphase (SEI), lithium metal battery.

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Acknowledgements

Publication history

Received: 01 May 2022
Revised: 29 January 2023
Accepted: 16 February 2023
Published: 27 February 2023
Issue date: March 2023

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© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

The authors are grateful for the financial support from the National Natural Science Foundation of China (Nos. 22075042 and 52102310), Shanghai Rising-Star Program (No. 22QA1400300), the Natural Science Foundation of Shanghai (No. 20ZR1401400), the Shanghai Scientific and Technological Innovation Project (No. 22520710100), the Fundamental Research Funds for the Central Universities, and the Donghua University (DHU) Distinguished Young Professor Program (No. LZB2021002).

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