Near-strain-free anode architecture enabled by interfacial diffusion creep for initial-anode-free quasi-solid-state batteries

Kwang Hee Kim, Myung-Jin Lee, Minje Ryu, Tae-Kyung Liu, Jung Hwan Lee, Changhoon Jung, Ju-Sik Kim () and Jong Hyeok Park ()
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Kwang Hee Kim: Yonsei University
Myung-Jin Lee: Samsung Advanced Institute of Technology
Minje Ryu: Yonsei University
Tae-Kyung Liu: Yonsei University
Jung Hwan Lee: Yonsei University
Changhoon Jung: Samsung Advanced Institute of Technology
Ju-Sik Kim: Samsung Advanced Institute of Technology
Jong Hyeok Park: Yonsei University

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Anode-free (or lithium-metal-free) batteries with garnet-type solid-state electrolytes are considered a promising path in the development of safe and high-energy-density batteries. However, their practical implementation has been hindered by the internal strain that arises from the repeated plating and stripping of lithium metal at the interlayer between the solid electrolyte and negative electrode. Herein, we utilize the titanium nitrate nanotube architecture and a silver-carbon interlayer to mitigate the anisotropic stress caused by the recurring formation of lithium deposition layers during the cycling process. The mixed ionic-electronic conducting nature of the titanium nitrate nanotubes effectively accommodates the entry of reduced Li into its free volume space via interfacial diffusion creep, achieving near-strain-free operation with nearly tenfold volume suppressing capability compared to a conventional Cu anode counterpart during the lithiation process. Notably, the fabricated Li6.4La3Zr1.7Ta0.3O12 (LLZTO)-based initial-anode-free quasi-solid-state battery full cell, coupled with an ionic liquid catholyte infused high voltage LiNi0.33Co0.33Mn0.33O2-based cathode with an areal capacity of 3.2 mA cm−2, exhibits remarkable room temperature (25 °C) cyclability of over 600 cycles at 1 mA cm−2 with an average coulombic efficiency of 99.8%.

Date: 2024
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DOI: 10.1038/s41467-024-48021-w

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