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<p>While solid electrolyte-excluded Si electrodes can form in situ lithiated monolithic structures with minimal side reactions, their poor performance at low operating pressures remains a formidable challenge for all-solid-state batteries. Herein, we propose an electrically conductive binder—poly(3,4-ethylenedioxythiophene):poly((styrene sulfonic acid)<sub><i>x</i></sub>-co-(maleic acid)<sub><i>y</i></sub>) (PEDOT:P(SS<sub><i>x</i></sub>-co-MA<sub><i>y</i></sub>))—that is scalable, fluorine-free, and water-processable. This binder offers sufficient e<sup>−</sup>-conductivity to eliminate carbon additives, while ensuring strong adhesion and electrochemical stability in contrast to conventional liquid electrolyte systems. Ex situ measurements reveal disrupted e-connectivity during delithiation at 5 MPa, resolved by employing PEDOT:P(SS<sub><i>x</i></sub>-co-MA<sub><i>y</i></sub>). The improved electrochemical performance of Si electrodes comprising PEDOT:P(SS<sub><i>x</i></sub>-co-MA<sub><i>y</i></sub>), compared with those using conventional polyvinylidene fluoride, is validated in (Li-In)&#xa0;|&#xa0;Li<sub>6</sub>PS<sub>5</sub>Cl | Si half cells and Si&#xa0;|&#xa0;Li<sub>6</sub>PS<sub>5</sub>Cl | LiNi<sub>0.70</sub>Co<sub>0.15</sub>Mn<sub>0.15</sub>O<sub>2</sub> full cells at 30 °C and 5 MPa, achieving 134 mAh g<sup>−1</sup> at 0.5 C with 86% capacity retention after 100 cycles. Finally, 233 mAh pouch-type Si || LiNi<sub>0.83</sub>Co<sub>0.12</sub>Mn<sub>0.05</sub>O<sub>2</sub> ASSBs are demonstrated, highlighting the potential of PEDOT:P(SS<sub><i>x</i></sub>-co-MA<sub><i>y</i></sub>) as a practical binder platform for high-energy ASSBs.</p>

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Electron-conductive binder for silicon negative electrode enabling low-pressure all-solid-state batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月5日

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  • Seunggoo Jun,
  • Minseok Jeong,
  • Boyeong Jang,
  • Seong-hyeon Jung,
  • Young Joon Park,
  • Yong Bae Song,
  • Jisoo Park,
  • Seungyun Jo,
  • Du Yeol Ryu,
  • Hanvin Kim,
  • Sungkyung Kim,
  • Jaewoo Lee,
  • Jeonghun Kim,
  • Yoon Seok Jung

摘要

While solid electrolyte-excluded Si electrodes can form in situ lithiated monolithic structures with minimal side reactions, their poor performance at low operating pressures remains a formidable challenge for all-solid-state batteries. Herein, we propose an electrically conductive binder—poly(3,4-ethylenedioxythiophene):poly((styrene sulfonic acid)x-co-(maleic acid)y) (PEDOT:P(SSx-co-MAy))—that is scalable, fluorine-free, and water-processable. This binder offers sufficient e−-conductivity to eliminate carbon additives, while ensuring strong adhesion and electrochemical stability in contrast to conventional liquid electrolyte systems. Ex situ measurements reveal disrupted e-connectivity during delithiation at 5 MPa, resolved by employing PEDOT:P(SSx-co-MAy). The improved electrochemical performance of Si electrodes comprising PEDOT:P(SSx-co-MAy), compared with those using conventional polyvinylidene fluoride, is validated in (Li-In) | Li6PS5Cl | Si half cells and Si | Li6PS5Cl | LiNi0.70Co0.15Mn0.15O2 full cells at 30 °C and 5 MPa, achieving 134 mAh g−1 at 0.5 C with 86% capacity retention after 100 cycles. Finally, 233 mAh pouch-type Si || LiNi0.83Co0.12Mn0.05O2 ASSBs are demonstrated, highlighting the potential of PEDOT:P(SSx-co-MAy) as a practical binder platform for high-energy ASSBs.