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<p>A key issue of all-solid-state rechargeable lithium batteries is the formation of a low-resistive electrode‒solid electrolyte interface. Since this problem begins with undesirable side reactions during the electrode‒solid electrolyte interface bonding process, the basic guidelines for suppressing side reactions need to be clarified. Here, we combine a typical Li<sup>+</sup>-conductive amorphous solid electrolyte, lithium phosphate, which exhibits various Li chemical potentials depending on the Li/P atomic ratio on the film surface, with c-axis oriented LiCoO<sub>2</sub> thin films. The lowest interfacial resistances of less than 10 Ω cm<sup>2</sup> are achieved within a certain range of Li/P atomic ratios. We clarify that interface bonding is classified as Li-insertion or Li-extraction types on the electrodes. The formation of appropriate ranges of Li-inserted or Li-extracted electrode states at the bonding interface is a major factor for attaining low-resistivity electrode–solid electrolyte interfaces and determining their appropriate combinations.</p><p></p>

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Chemical design rules for low-resistivity electrode–electrolyte interfaces in all-solid-state lithium batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月9日

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  • Morihiro Maruno,
  • Futa Nakayama,
  • Yasuhiro Suzuki,
  • Miyuki Sakakura,
  • Tsuyoshi Ohnishi,
  • Yuki Nomura,
  • Koji Hiraoka,
  • Kazuo Yamamoto,
  • Takeshi Yajima,
  • Yasutoshi Iriyama

摘要

A key issue of all-solid-state rechargeable lithium batteries is the formation of a low-resistive electrode‒solid electrolyte interface. Since this problem begins with undesirable side reactions during the electrode‒solid electrolyte interface bonding process, the basic guidelines for suppressing side reactions need to be clarified. Here, we combine a typical Li+-conductive amorphous solid electrolyte, lithium phosphate, which exhibits various Li chemical potentials depending on the Li/P atomic ratio on the film surface, with c-axis oriented LiCoO2 thin films. The lowest interfacial resistances of less than 10 Ω cm2 are achieved within a certain range of Li/P atomic ratios. We clarify that interface bonding is classified as Li-insertion or Li-extraction types on the electrodes. The formation of appropriate ranges of Li-inserted or Li-extracted electrode states at the bonding interface is a major factor for attaining low-resistivity electrode–solid electrolyte interfaces and determining their appropriate combinations.