Efficient diffusion of superdense lithium via atomic channels for dendrite-free lithium–metal batteries

The non-uniform aggregation of fast-diffused Li on an anode surface would aggravate its tip-effect-induced nucleation/growth, leading to the notorious dendrite growth in Li metal batteries (LMBs). Tuning the Li diffusion on the anode surface has been regarded previously as a mainstream method to ind...

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Published in:Energy & environmental science 2022-01, Vol.15 (1), p.196-205
Main Authors: Zhou, Shiyuan, Chen, Weixin, Shi, Jie, Li, Gen, Pei, Fei, Liu, Sangui, Ye, Weibin, Xiao, Liangping, Wang, Ming-Sheng, Wang, Dan, Qiao, Yu, Huang, Ling, Xu, Gui-Liang, Liao, Hong-Gang, Chen, Jian-Feng, Amine, Khalil, Sun, Shi-Gang
Format: Article
Language:English
Subjects:
Anode effect
Batteries
Bulk density
Cathodes
Channels
Dendritic structure
Density functional theory
Diffusion
Diffusion rate
Energy storage
Lithium
Lithium batteries
Molecular dynamics
Nucleation
Storage systems
Transmission electron microscopy
Tunnel construction
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Summary:The non-uniform aggregation of fast-diffused Li on an anode surface would aggravate its tip-effect-induced nucleation/growth, leading to the notorious dendrite growth in Li metal batteries (LMBs). Tuning the Li diffusion on the anode surface has been regarded previously as a mainstream method to induce its uniform deposition, while the diffusion of Li in the anode bulk is usually ignored. Here, conceptually different from the classic surface modification, we propose a molecular tunnelling strategy to construct atomic channels in graphite bulk, which enables the fast diffusion of superdense Li. Density functional theory calculations and ab initio molecular dynamics simulations prove that the bulk diffusion through atomic channels could become a new and dominating path. Its reversible and efficient diffusion has been further visualized by in situ transmission electron microscopy. As a result, when coupled with high-loading LiFePO 4 cathodes (20 mg cm −2 ), a high areal capacity and 100% capacity retention are achieved over 370 cycles. Through this work a new strategy is developed based on the bulk-diffusion of superdense Li for dendrite-free LMBs, which can be pervasive in other high-performance energy storage systems.
ISSN:1754-5692
1754-5706
DOI:10.1039/D1EE02205A