Interface engineering enabling thin lithium metal electrodes down to 0.78 μm for garnet-type solid-state batteries.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 39548085.
- Also identified by DOI 10.1038/s41467-024-54234-w and PMC identifier 11568204.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
Controllable engineering of thin lithium (Li) metal is essential for increasing the energy density of solid-state batteries and clarifying the interfacial evolution mechanisms of a lithium metal negative electrode. However, fabricating a thin lithium electrode faces significant challenges due to the fragility and high viscosity of Li metal. Herein, through facile treatment of Ta-doped Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZTO) with trifluoromethanesulfonic acid, its surface Li<sub>2</sub>CO<sub>3</sub> species is converted into a lithiophilic layer with LiCF<sub>3</sub>SO<sub>3</sub> and LiF components. It enables the thickness control of Li metal negative electrodes, ranging from 0.78 μm to 30 μm. Quasi-solid-state lithium-metal battery with an optimized 7.54 μm-thick lithium metal negative electrode, a commercial LiNi<sub>0.83</sub>Co<sub>0.11</sub>Mn<sub>0.06</sub>O<sub>2</sub> positive electrode, and a negative/positive electrode capacity ratio of 1.1 shows a 500 cycles lifespan with a final discharge specific capacity of 99 mAh g<sup>-1</sup> at 2.35 mA cm<sup>-2</sup> and 25 °C. Through multi-scale characterizations of the thin lithium negative electrode, we clarify the multi-dimensional compositional evolution and failure mechanisms of lithium-deficient and -rich regions (0.78 μm and 7.54 μm), on its surface, inside it, or at the Li/LLZTO interface.