Garnet-Type Solid-State Electrolyte with Tailored Lithium Compatibility for High Performance All-Solid-State Lithium Batteries.
basic_science · Level V
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- Record sourced from PubMed, PMID 41367167.
- Also identified by DOI 10.1002/adma.202509828.
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Abstract
Garnet-type Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) solid-state electrolyte (SSE) demonstrates appealing ionic conductivity for all-solid-state battery applications. However, the interfacial compatibility between LLZO and the lithium electrode is yet to be addressed for the deployment of practical batteries at scale. Herein, tailored cubic-phase garnet-type Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub> <sub>-x</sub>Sc<sub>x</sub>O<sub>12</sub> <sub>-x</sub>F<sub>x</sub> (LLZSOF-x, x = 0-0.20) SSEs are designed, which features high lithium content and superior compatibility with the lithium metal electrode. The strong binding of fluorine dopant with octahedral lithium ions significantly inhibits Li⁺/H⁺ exchange, thus achieving intimate interfacial contact between composition-optimized Li<sub>7</sub>La<sub>3</sub>Zr<sub>1.85</sub>Sc<sub>0.15</sub>O<sub>11.85</sub>F<sub>0.15</sub> (LLZSOF-0.15) and lithium electrode. Meanwhile, scandium substitution increases lithium content to 7.0, leading to improved reduction stability toward lithium metal. The LLZSOF-0.15 based symmetric cell yields high critical current density of 1.9 mA cm<sup>-2</sup>, which meets the practical requirements for solid-state batteries. And LLZSOF-0.15 based all-solid-state lithium metal batteries show excellent cyclability, with high-capacity retention of 83.2% over 240 cycles for LiFePO<sub>4</sub> and 84.1% over 140 cycles for LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM) (0.5 C). Li/LLZSOF-0.15/NCM pouch cells maintain over 99.5% Coulombic efficiency and 94.9% capacity retention after 120 cycles at 0.5 C. This study establishes a material design approach for developing garnet SSEs with superior interfacial compatibility, promoting the deployment of advanced all-solid-state batteries at scale.