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<p>Garnet-type electrolytes are pivotal for developing safe, high-capacity all-solid-state lithium batteries (ASSLBs), yet their advancement is critically impeded by the poor physical contact and consequent high impedance at the lithium metal anode/electrolyte interface. Herein, we report a facile yet effective interface engineering strategy by modifying the surface tension of molten lithium. Introducing a mere 0.1 wt% of gallium (Ga) into the Li anode—a quantity that negligibly affects its theoretical specific capacity—dramatically enhances its wettability against the garnet electrolyte. This modification forges an intimate and stable Li-Ga/garnet interface, achieving an exceptionally low area-specific resistance (ASR) of 5.5 Ω cm<sup>2</sup> at 30&#xa0;°C. Consequently, symmetric batteries with the modified anode demonstrate a high critical current density (CCD) of 1.15&#xa0;mA cm<sup>-2</sup> and remarkable cycling stability, operating for over 1000&#xa0;h at 0.3&#xa0;mA cm<sup>-2</sup> without failure. This work demonstrates that trace-element alloying is a highly effective strategy for resolving the interfacial challenges in garnet-based ASSLBs, paving the way for their practical implementation.</p>

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Trace Ga-doped interface engineering for stable lithium anode/LLZO integration in quasi-solid-state batteries

  • 期刊论文

  • 发表日期：

    2025年12月13日

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  • Shangbin Song,
  • Jiaxu Zhang,
  • Shiyu Cao,
  • Zhangmancang Xu,
  • Minghao Ye,
  • Lianmeng Zhang,
  • Gangjian Tan,
  • Fei Chen

摘要

Garnet-type electrolytes are pivotal for developing safe, high-capacity all-solid-state lithium batteries (ASSLBs), yet their advancement is critically impeded by the poor physical contact and consequent high impedance at the lithium metal anode/electrolyte interface. Herein, we report a facile yet effective interface engineering strategy by modifying the surface tension of molten lithium. Introducing a mere 0.1 wt% of gallium (Ga) into the Li anode—a quantity that negligibly affects its theoretical specific capacity—dramatically enhances its wettability against the garnet electrolyte. This modification forges an intimate and stable Li-Ga/garnet interface, achieving an exceptionally low area-specific resistance (ASR) of 5.5 Ω cm2 at 30 °C. Consequently, symmetric batteries with the modified anode demonstrate a high critical current density (CCD) of 1.15 mA cm-2 and remarkable cycling stability, operating for over 1000 h at 0.3 mA cm-2 without failure. This work demonstrates that trace-element alloying is a highly effective strategy for resolving the interfacial challenges in garnet-based ASSLBs, paving the way for their practical implementation.