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<p>Aqueous Zn-ion batteries encounter significant challenges, including unstable electrolyte interfaces and dendrite formation, which curtail their cycle life and metal utilization. Here, we present a self-separating biphasic electrolyte through phase separation of poly (3,4-ethylenedioxythiophene): poly (styrenesulfonic acid) (PEDOT:PSS) conductive polymers in Zn sulfate solution driven by a mechanical shear-ionic crosslinking process. The negatively charged sulfonic groups in PSS disrupt the hydrogen-bonding network of bulk electrolyte and remodel solvation structure of Zn<sup>2+</sup> ions, enhancing ionic transfer kinetics and facilitating desolvation. Meanwhile, the insoluble PEDOT fibers with continuous conjugated thiophene ring together with sulfonic groups in PSS spontaneously adhere to the electrode surface, establishing a robust electron-rich interphase that regulates electric double layer thickness, promotes uniform Zn deposition and repels sulfate ions. Consequently, this electrolyte allows Zn anodes to achieve exceptional stability and longevity even at larger depths of discharge (68.4% and 94.1%) and delivers outstanding cyclability exceeding 10,000 cycles in Zn||V<sub>2</sub>O<sub>5</sub> full cells.</p>

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Self-Separating Biphasic Electrolyte Enables High-Performance Aqueous Zinc-Ion Batteries via Electron-Enriched Interphase Engineering

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年5月12日

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  • Chengwu Yang,
  • Pattaraporn Woottapanit,
  • Qizhi Hou,
  • Zhiqiang Dai,
  • Wanwisa Limphirat,
  • Jiaqian Qin,
  • Xinyu Zhang

摘要

Aqueous Zn-ion batteries encounter significant challenges, including unstable electrolyte interfaces and dendrite formation, which curtail their cycle life and metal utilization. Here, we present a self-separating biphasic electrolyte through phase separation of poly (3,4-ethylenedioxythiophene): poly (styrenesulfonic acid) (PEDOT:PSS) conductive polymers in Zn sulfate solution driven by a mechanical shear-ionic crosslinking process. The negatively charged sulfonic groups in PSS disrupt the hydrogen-bonding network of bulk electrolyte and remodel solvation structure of Zn2+ ions, enhancing ionic transfer kinetics and facilitating desolvation. Meanwhile, the insoluble PEDOT fibers with continuous conjugated thiophene ring together with sulfonic groups in PSS spontaneously adhere to the electrode surface, establishing a robust electron-rich interphase that regulates electric double layer thickness, promotes uniform Zn deposition and repels sulfate ions. Consequently, this electrolyte allows Zn anodes to achieve exceptional stability and longevity even at larger depths of discharge (68.4% and 94.1%) and delivers outstanding cyclability exceeding 10,000 cycles in Zn||V2O5 full cells.