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Synergistic effect of embossed Cu current collector and potassium nitrate for achieving dense lithium deposition and improving cycle life in anode-free Li metal batteries

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Abstract

Anode-free lithium metal batteries (AFLMB) operate solely with lithium (Li) in the lithiated cathode, eliminating the mass and volume of the anode to maximize energy density of the battery. However, uneven Li deposition can lead to the formation of Li dendrites, hindering practical applications due to issues like solid electrolyte interphase (SEI) breakage and low coulombic efficiency (CE). To address these challenges, we investigated the synergistic effect of applying a 3D-structured current collector (CC) and KNO3 for Li deposition control. We fabricated an embossed Cu CC with a 3D structure using a copper nanoparticle (Cu NP) slurry and intense pulsed light (IPL) sintering techniques. When KNO3 electrolyte additives were used in conjunction with the manufactured 3D embossed Cu, we observed a significant improvement in cycle life. The KNO3 additive prevented the top plating of Li through an electrostatic shielding effect, while the anion contributed to dense Li deposition by forming a stable SEI layer, such as Li3N. Consequently, the combination of embossed Cu and KNO3 enabled thick and compact Li deposition, reducing Li loss during the plating and stripping processes and thereby improving the lifespan of the cell. In AFLMB matched with NCM811, capacity retention after 50 cycles increased to 52%, compared to 0.8% in the absence of electrolyte additives, demonstrating stable operation even after more than 100 cycles. Therefore, combining a thin, 3D-structured CC with an electrolyte additive capable of controlling Li deposition presents a promising strategy for enhancing the practical use of carbonate electrolyte-based AFLMB through synergistic effects.

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Data availability

The authors declare that the data supporting the findings of this study are available within the paper and its Supplementary Information files. Should any raw data files be needed in another format they are available from the corresponding author upon reasonable request.

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Acknowledgements

This research was supported by grants from the Basic Science Research Program through the National Research Foundation of Korea (NRF), funded by the Ministry of Education (2022R1A2C2010451), and by a grant funded by the Ministry of Trade, Industry and Energy (00155725).

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Authors and Affiliations

  1. Department of Organic and Nano Engineering, Hanyang University, 222 Wangsimni-ro, Seongdong-gu, Seoul, 04763, Republic of Korea

    Suhyun Ahn, Sucheol Kim & Heejoon Ahn

  2. Department of Battery Engineering, Hanyang University, 222 Wangsimni-ro, Seongdong-gu, Seoul, 04763, Republic of Korea

    Hyeonjun Song & Heejoon Ahn

  3. Human-Tech Convergence Program, Department of Organic and Nano Engineering, Hanyang University, 222 Wangsimni-ro, Seongdong-gu, Seoul, 04763, Republic of Korea

    Sucheol Kim & Heejoon Ahn

  4. Department of Mechanical Engineering, Hanyang University, 222 Wangsimni-ro, Seongdong-gu, Seoul, 04763, Republic of Korea

    Hojae Lee & Young-Beom Kim

  5. Jeong Gwang Co., LTD, 861-41, Dongsan-ri, Cheonbuk-Myeon, Gyeongju-si, Gyeongsangbuk-do, 38039, Republic of Korea

    Kihun Jang & Minsoo Ha

  6. Institute of Nano Science and Technology, Hanyang University, 222 Wangsimni-ro, Seongdong-gu, Seoul, 04763, Republic of Korea

    Young-Beom Kim & Heejoon Ahn

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Ahn, S., Song, H., Kim, S. et al. Synergistic effect of embossed Cu current collector and potassium nitrate for achieving dense lithium deposition and improving cycle life in anode-free Li metal batteries. J. Korean Ceram. Soc. 61, 267–278 (2024). https://doi.org/10.1007/s43207-023-00354-w

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