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Nano Research 2021, 14(10): 3585-3597 https://doi.org/10.1007/s12274-021-3643-1
Research Article | Open Access | Issue | Published: 09 July 2021

Nano-channel-based physical and chemical synergic regulation for dendrite-free lithium plating

Show Author's Information Qiang Guo1,2,  Wei Deng1,  Shengjie Xia1,  Zibo Zhang1,  Fei Zhao1,  Binjie Hu2,  Sasa Zhang1,  Xufeng Zhou1( ),  George Zheng Chen3( ),  Zhaoping Liu1( )
Key Laboratory of Graphene Technologies and Applications of Zhejiang Province and Advanced Li-ion Battery Engineering Laboratory of Zhejiang Province,Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences (CAS),Ningbo,315201,China;
Department of Chemical and Environmental Engineering,Faculty of Science and Engineering, University of Nottingham,Ningbo,315100,China;
Department of Chemical and Environmental Engineering, Faculty of Engineering,University of Nottingham,Nottingham, NG7, 2RD, UK,
Keywords:
carbon nitride, porous structure, Debye length, lithiophilic coating, Li negative electrode
Topics:
Lithium batteries
Cite this article:
Guo Q, Deng W, Xia S, et al. Nano-channel-based physical and chemical synergic regulation for dendrite-free lithium plating. Nano Research, 2021, 14(10): 3585-3597. https://doi.org/10.1007/s12274-021-3643-1
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Abstract Full text Electronic supplementary material About this article

Uncontrollable dendrite growth resulting from the non-uniform lithium ion (Li+) flux and volume expansion in lithium metal (Li) negative electrode leads to rapid performance degradation and serious safety problems of lithium metal batteries. Although N-containing functional groups in carbon materials are reported to be effective to homogenize the Li+ flux, the effective interaction distance between lithium ions and N-containing groups should be relatively small (down to nanometer scale) according to the Debye length law. Thus, it is necessary to carefully design the microstructure of N-containing carbon materials to make the most of their roles in regulating the Li+ flux. In this work, porous carbon nitride microspheres (PCNMs) with abundant nanopores have been synthesized and utilized to fabricate a uniform lithiophilic coating layer having hybrid pores of both the nano- and micrometer scales on the Cu/Li foil. Physically, the three-dimensional (3D) porous framework is favorable for absorbing volume changes and guiding Li growth. Chemically, this coating layer can render a suitable interaction distance to effectively homogenize the Li+ flux and contribute to establishing a robust and stable solid electrolyte interphase (SEI) layer with Li-F, Li-N, and Li-O-rich contents based on the Debye length law. Such a physical-chemical synergic regulation strategy using PCNMs can lead to dendrite-free Li plating, resulting in a low nucleation overpotential and stable Li plating/stripping cycling performance in both the Li‖Cu and the Li‖Li symmetric cells. Meanwhile, a full cell using the PCNM coated Li foil negative electrode and a LiFePO4 positive electrode has delivered a high capacity retention of ~ 80% after more than 200 cycles at 1 C and achieved a remarkable rate capability. The pouch cell fabricated by pairing the PCNM coated Li foil negative electrode with a NCM 811 positive electrode has retained ~ 73% of the initial capacity after 150 cycles at 0.2 C.


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Abstract
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Electronic supplementary material
About this article

Nano-channel-based physical and chemical synergic regulation for dendrite-free lithium plating

Show Author's information Qiang Guo1,2, Wei Deng1, Shengjie Xia1, Zibo Zhang1, Fei Zhao1, Binjie Hu2, Sasa Zhang1, Xufeng Zhou1( ), George Zheng Chen3( ), Zhaoping Liu1( )
Key Laboratory of Graphene Technologies and Applications of Zhejiang Province and Advanced Li-ion Battery Engineering Laboratory of Zhejiang Province,Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences (CAS),Ningbo,315201,China;
Department of Chemical and Environmental Engineering,Faculty of Science and Engineering, University of Nottingham,Ningbo,315100,China;
Department of Chemical and Environmental Engineering, Faculty of Engineering,University of Nottingham,Nottingham, NG7, 2RD, UK,

Abstract

Uncontrollable dendrite growth resulting from the non-uniform lithium ion (Li+) flux and volume expansion in lithium metal (Li) negative electrode leads to rapid performance degradation and serious safety problems of lithium metal batteries. Although N-containing functional groups in carbon materials are reported to be effective to homogenize the Li+ flux, the effective interaction distance between lithium ions and N-containing groups should be relatively small (down to nanometer scale) according to the Debye length law. Thus, it is necessary to carefully design the microstructure of N-containing carbon materials to make the most of their roles in regulating the Li+ flux. In this work, porous carbon nitride microspheres (PCNMs) with abundant nanopores have been synthesized and utilized to fabricate a uniform lithiophilic coating layer having hybrid pores of both the nano- and micrometer scales on the Cu/Li foil. Physically, the three-dimensional (3D) porous framework is favorable for absorbing volume changes and guiding Li growth. Chemically, this coating layer can render a suitable interaction distance to effectively homogenize the Li+ flux and contribute to establishing a robust and stable solid electrolyte interphase (SEI) layer with Li-F, Li-N, and Li-O-rich contents based on the Debye length law. Such a physical-chemical synergic regulation strategy using PCNMs can lead to dendrite-free Li plating, resulting in a low nucleation overpotential and stable Li plating/stripping cycling performance in both the Li‖Cu and the Li‖Li symmetric cells. Meanwhile, a full cell using the PCNM coated Li foil negative electrode and a LiFePO4 positive electrode has delivered a high capacity retention of ~ 80% after more than 200 cycles at 1 C and achieved a remarkable rate capability. The pouch cell fabricated by pairing the PCNM coated Li foil negative electrode with a NCM 811 positive electrode has retained ~ 73% of the initial capacity after 150 cycles at 0.2 C.

Keywords: carbon nitride, porous structure, Debye length, lithiophilic coating, Li negative electrode

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Publication history

Received: 15 March 2021
Revised: 24 May 2021
Accepted: 02 June 2021
Published: 09 July 2021
Issue date: October 2021

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© The Author(s) 2021

Acknowledgements

Acknowledgements

This work was supported by the National Key R & D Program of China (No. 2016YFF0204302), the National Natural Science Foundation of China (Nos. 51872305 and 52001320), and S & T Innovation 2025 Major Special Programme of Ningbo (No. 2018B10081). The authors also thank Doctoral Training Partnership Programme provided by University of Nottingham Ningbo, China and Ningbo Institute of Materials Technology & Engineering, Chinese Academy of Sciences.

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