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<p>All-solid-state batteries (ASSBs) are considered to be the most promising candidates for improving battery safety and energy density. Sulfide electrolytes have a narrow electrochemical window, which hinders their applications coupled with high-voltage cathodes. Halide electrolytes with high-voltage endurance can help solve this problem. Herein, the combination of spraying and slurry-coating methods was adopted as a practical route to process a free-standing Li<sub>6</sub>PS<sub>5</sub>Cl (LPSCl) asymmetrical electrolyte membrane (19.23 Ω cm<sup>2</sup>, 75 µm) decorated with a 10 µm Li<sub>3</sub>InCl<sub>6</sub> (LICl) layer. The LICl-LPSCl asymmetrical electrolyte membranes enhanced the high-voltage stabilities to match those of LiNi<sub>0.83</sub>Co<sub>0.11</sub>Mn<sub>0.06</sub>O<sub>2</sub> (NCM811) and Li<sub>1.2</sub>Ni<sub>0.13</sub>Co<sub>0.13</sub>Mn<sub>0.54</sub>O<sub>2</sub> (LRMO) cathodes. The NCM811∣LICl-LPSCl∣nSi ASSB achieved an initial coulombic efficiency (ICE) of 85.13% and a capacity retention of 77.16% after 200 cycles. Compared with the LPSCl membrane, the LICl-LPSCl membrane displayed high stability with the LRMO cathode as the charging cut-off voltage increased to 4.7 V, which improved the initial charge capacity from 143 to 270 mAh g<sup>−1</sup> and achieved stable cycling of 160 mAh g<sup>−1</sup> at 0.5 C. Additionally, we attempted continuous LICl-LPSCl membrane production and utilized the product to fabricate a pouch-type ASSB based on LRMO. The fabrication of the LICl-LPSCl electrolyte membrane demonstrated its potential for controllable and industry-adaptable applications in ASSBs.</p>

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Scalable preparation of asymmetrical bilayer sulfide/halide electrolyte membranes for all-solid-state batteries with high voltage

  • 期刊论文

  • 发表日期：

    2025年2月14日

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  • Shenghao Jing,
  • Yanchen Liu,
  • Yang Lu,
  • Hanzhou Liu,
  • Yang Liu,
  • Siliang Liu,
  • Zongliang Zhang,
  • Fangyang Liu

摘要

All-solid-state batteries (ASSBs) are considered to be the most promising candidates for improving battery safety and energy density. Sulfide electrolytes have a narrow electrochemical window, which hinders their applications coupled with high-voltage cathodes. Halide electrolytes with high-voltage endurance can help solve this problem. Herein, the combination of spraying and slurry-coating methods was adopted as a practical route to process a free-standing Li6PS5Cl (LPSCl) asymmetrical electrolyte membrane (19.23 Ω cm2, 75 µm) decorated with a 10 µm Li3InCl6 (LICl) layer. The LICl-LPSCl asymmetrical electrolyte membranes enhanced the high-voltage stabilities to match those of LiNi0.83Co0.11Mn0.06O2 (NCM811) and Li1.2Ni0.13Co0.13Mn0.54O2 (LRMO) cathodes. The NCM811∣LICl-LPSCl∣nSi ASSB achieved an initial coulombic efficiency (ICE) of 85.13% and a capacity retention of 77.16% after 200 cycles. Compared with the LPSCl membrane, the LICl-LPSCl membrane displayed high stability with the LRMO cathode as the charging cut-off voltage increased to 4.7 V, which improved the initial charge capacity from 143 to 270 mAh g−1 and achieved stable cycling of 160 mAh g−1 at 0.5 C. Additionally, we attempted continuous LICl-LPSCl membrane production and utilized the product to fabricate a pouch-type ASSB based on LRMO. The fabrication of the LICl-LPSCl electrolyte membrane demonstrated its potential for controllable and industry-adaptable applications in ASSBs.