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Research Article

Regulating Li transport in Li-magnesium alloy for dendrite free Li metal anode

Jinxi Wang1, Yadong Ye1, Hongmin Zhou2, Wei Zhang1, Zhaowei Sun1, Jiawen Zhu1, Hongchang Jin1, Huanyu Xie1, Haoliang Huang3, Yi Cui4, Rong Huang4, Zezhong Li5, Song Jin1( ), Hengxing Ji1( )
Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Applied Chemistry, University of Science and Technology of China, Hefei 230026, China
Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, China
Hefei National Laboratory for Physical Sciences at the Microscale and Anhui Laboratory of Advanced Photon Science and Technology, University of Science and Technology of China, Hefei 230026, China
Vacuum Interconnected Nanotech Workstation (NANO-X), Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO), Suzhou 215123, China
School of Earth and Space Sciences, University of Science and Technology of China, Hefei 230026, China
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Graphical Abstract

Here we find the difference in the diffusion coefficient of Li atoms on solid-solution-based metal alloy phases is a major contributor to the different deposition behaviors. The low Li atom diffusion coefficient of Li-Mg alloy shows a preferential Li accumulation on the upper surface rather than the inward-growth plating of Li atoms into alloy foil. By the process of secondary recrystallization, we improve the diffusion coefficient of Li atoms in Li-Mg alloy that facilitate the inward transfer.

Abstract

Li metal has become a strong candidate for anode due to its high theoretical specific capacity and lowest electrochemical potential. However, the poor reversibility caused by continuous chemical and electrochemical degradation hinders the practical application of Li metal. Solid-solution-based metal alloy phases have been proposed as hosts for regulating the non-dendrite electrodeposition, but the fundamental understanding remains unclear due to the drastically different deposition behaviors of Li on them. Here we found the difference in the diffusion coefficient of Li atoms on solid-solution-based metal alloy phases (Li-Mg and Li-Ag alloys) was a major contributor to the different deposition behaviors. The low Li atom diffusion coefficient of Li-Mg alloy showed a preferential Li accumulation on the upper surface rather than the inward-growth plating of Li atoms into alloy foil in Li-Ag alloy. By the process of secondary recrystallization, we improved the diffusion coefficient of Li atoms in Li-Mg alloy that facilitates the inward transfer rather than surface plating of Li atoms. In this case, the recrystallized Li-Mg alloy underwent a solid-solution phase change in the delithiation–lithiation cycles which yielded a high Coulombic efficiency of 99.3% with a reversible gravimetric capacity of 2,874 mAh·g−1 and superior cycling stability over 5,000 h without dendrite growth.

Keywords

Li-Mg alloysolid solutionrecrystallizationlithium metal anodediffusion coefficient

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Nano Research
Volume 16 Issue 6,
June 2023
Pages 8338-8344
DOI: 10.1007/s12274-022-5044-5
Cite this article:
Wang J, Ye Y, Zhou H, et al. Regulating Li transport in Li-magnesium alloy for dendrite free Li metal anode. Nano Research, 2023, 16(6): 8338-8344. https://doi.org/10.1007/s12274-022-5044-5
Topics:
Storage (materials)
Part of a topical collection:
Conversion Reaction Lithium Metal Batteries

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Received: 10 June 2022
Revised: 31 August 2022
Accepted: 13 September 2022
Published: 24 October 2022
© Tsinghua University Press 2022
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