Electron-conductive binder for silicon negative electrode enabling low-pressure all-solid-state batteries.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 41350528.
- Also identified by DOI 10.1038/s41467-025-66851-0 and PMC identifier 12774888.
- Licence recorded as CC BY-NC-ND.
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Abstract
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>x</sub>-co-(maleic acid)<sub>y</sub>) (PEDOT:P(SS<sub>x</sub>-co-MA<sub>y</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>x</sub>-co-MA<sub>y</sub>). The improved electrochemical performance of Si electrodes comprising PEDOT:P(SS<sub>x</sub>-co-MA<sub>y</sub>), compared with those using conventional polyvinylidene fluoride, is validated in (Li-In) | Li<sub>6</sub>PS<sub>5</sub>Cl | Si half cells and Si | 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>x</sub>-co-MA<sub>y</sub>) as a practical binder platform for high-energy ASSBs.