Electron Percolating Shielded Interlayer Enabling Ultrastable All-Solid-State Lithium Metal Batteries.
basic_science · Level V
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- Record sourced from PubMed, PMID 41251518.
- Also identified by DOI 10.1002/adma.202515687.
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Abstract
The electron percolation of grain boundaries in Li<sub>6.4</sub>La<sub>3</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>12</sub> (LLZTO) induces internal lithium deposition and penetration, causing short circuits of all-solid-state batteries, which has become a significant obstacle hindering the practical application of LLZTO. In this work, an electron-percolating shielded interface constructing strategy is proposed between LLZTO and lithium metal (Li) to simultaneously suppress the Li dendrite growth at both the interface and within the LLZTO electrolyte. A Poly[bis(4-phenyl)(2,4,6-triMethylphenyl)aMine] (PTAA)/SnO<sub>2</sub> (PS) bilayer is therefore designed between LLZTO and Li metal (LLZTO-PS|Li), where the hole-rich PTAA and electron-rich SnO<sub>2</sub> generate a reverse electric field that effectively blocks the electron leakage, thereby reducing the electronic conductivity of LLZTO and preventing its internal dendrite formation. Furthermore, the smooth and compact PTAA/SnO<sub>2</sub> coating significantly enhances interfacial contact and equalizes the interfacial potential to promote a uniform Li plating. As a result, the Li|LLZTO-PS|Li symmetric battery achieves stable cycling for over 5000 h at 0.1 mA cm<sup>-2</sup> and 2500 h at 0.5 mA cm<sup>-2</sup>. The Li|LLZTO-PS|LiFePO<sub>4</sub> full battery demonstrates 86.2% capacity after 2000 cycles at 1 C. This study presents a novel interfacial engineering strategy for enhancing the performance and durability of garnet-based all-solid-state lithium-metal batteries.