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<p>The dry-process is a sustainable and promising fabrication method for all-solid-state batteries by eliminating solvents. However, a pragmatic fabrication design for thin and robust solid-state electrolyte (SSE) layers has not been established. Herein, we report a dry-process approach that enhances mechanical stability of SSE layers from film fabrication to cell operation. By co-rolling thick SSE and positive electrode feeds, a uniform, thin SSE layer (50 µm) and a high loading positive electrode layer (5 mAh cm<sup>−2</sup>) with high active material ratio (80 wt%) are simultaneously achieved. This SSE-positive electrode integrated film exhibits enhanced physical properties and cyclability (&gt; 80% retention after 500 cycles) at low stack pressure (2 MPa) compared to the freestanding counterparts, attributed to reinforced and intimate SSE-positive electrode interface constructed during co-rolling process. Additionally, an all-solid-state pouch cell with high stack-level specific energy (310 Wh kg<sup>−1</sup>) and energy density (805 Wh L<sup>−1</sup>) operating at 30 °C and 5 MPa is demonstrated.</p>

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Robust interface and reduced operation pressure enabled by co-rolling dry-process for stable all-solid-state batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年5月6日

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  • Dong Ju Lee,
  • Yuju Jeon,
  • Jung-Pil Lee,
  • Lanshuang Zhang,
  • Ki Hwan Koh,
  • Feng Li,
  • Anthony U. Mu,
  • Junlin Wu,
  • Yu-Ting Chen,
  • Seamus McNulty,
  • Wei Tang,
  • Marta Vicencio,
  • Dapeng Xu,
  • Jiyoung Kim,
  • Zheng Chen

摘要

The dry-process is a sustainable and promising fabrication method for all-solid-state batteries by eliminating solvents. However, a pragmatic fabrication design for thin and robust solid-state electrolyte (SSE) layers has not been established. Herein, we report a dry-process approach that enhances mechanical stability of SSE layers from film fabrication to cell operation. By co-rolling thick SSE and positive electrode feeds, a uniform, thin SSE layer (50 µm) and a high loading positive electrode layer (5 mAh cm−2) with high active material ratio (80 wt%) are simultaneously achieved. This SSE-positive electrode integrated film exhibits enhanced physical properties and cyclability (> 80% retention after 500 cycles) at low stack pressure (2 MPa) compared to the freestanding counterparts, attributed to reinforced and intimate SSE-positive electrode interface constructed during co-rolling process. Additionally, an all-solid-state pouch cell with high stack-level specific energy (310 Wh kg−1) and energy density (805 Wh L−1) operating at 30 °C and 5 MPa is demonstrated.