Magnetically oriented nanosheet interlayer for dynamic regeneration in lithium metal batteries

Journal Article · 23 October 2024 · Proceedings of the National Academy of Sciences of the United States of America

DOI: https://doi.org/10.1073/pnas.2413739121 · OSTI ID:2473450

Ju, Zhengyu  ^[1]; Zheng, Tianrui ^[1]; Zhang, Bowen ^[1]; Dolocan, Andrei ^[2]; Marschilok, Amy C.  ^[3]; Takeuchi, Esther S. ^[3]; Takeuchi, Kenneth J.  ^[3]; Yu, Guihua  ^[1]

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1. Materials Science and Engineering Program and Walker Department of Mechanical Engineering, The University of Texas at Austin, Austin, TX 78712
2. Texas Materials Institute, University of Texas at Austin, Austin, TX 78712
3. Institute of Energy: Environment, Sustainability and Equity, Stony Brook University, Stony Brook, NY 11794, Department of Chemistry, Stony Brook University, Stony Brook, NY 11794, Interdisciplinary Science Department, Brookhaven National Laboratory, Upton, NY 11973, Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, NY 11794

Lithium (Li) metal has been recognized as a promising anode to advance the energy density of current Li-based batteries. However, the growth of the solid–electrolyte interphase (SEI) layer and dendritic Li microstructure pose significant challenges for the long-term operation of Li metal batteries (LMBs). Herein, we propose the utilization of a suspension electrolyte with dispersed magnetically responsive nanosheets whose orientation can be manipulated by an external magnetic field during cell operation for realizing in situ regeneration in LMBs. The regeneration mechanism arises from the redistribution of the ion flux and the formation of an inorganic-rich SEI for uniform and compact Li deposition. With the magnetic-field-induced regeneration process, we show that a Li||Li symmetric cell stably operates for 350 h at 2 mA cm ⁻² and 2 mA h cm ⁻² , ~5 times that of the cell with the pristine electrolyte. Furthermore, the cycling stability can be significantly extended in the Li||NMC full cell of 3 mA h cm ⁻² , showing a capacity retention of 67% after 500 cycles at 1C. The dynamic Li metal regeneration demonstrated here could bring useful design considerations for reviving the operating cells for achieving high-energy, long-duration battery systems.

• Sponsoring Organization: USDOE
• Grant/Contract Number: SC0012673
• OSTI ID: 2473450
• Journal Information: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 44 Vol. 121; ISSN 0027-8424
• Publisher: Proceedings of the National Academy of SciencesCopyright Statement
• Country of Publication: United States
• Language: English