Interface Engineering for Constructing Air-Stable and Lithiophilic Garnet-Type Solid Electrolytes.

Zhang, Sidong; Jia, Meiqi; Guo, Sijie; Grundish, Nicholas S; Cao, An-Min; Li, Yutao · Nano Lett · 2025

basic_science · Level V

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Abstract

Garnet-type solid electrolytes (SEs) exhibit high ionic conductivity, a wide electrochemical window, and lithium stability, making them ideal for solid-state Li metal batteries. However, their air sensitivity leads to Li<sub>2</sub>CO<sub>3</sub> formation, causing poor Li wettability, high interfacial resistance, and dendrite growth. To address this, Mg<sub>3</sub>(PO<sub>4</sub>)<sub>2</sub> is coated via a wet chemistry method, converting Li<sub>2</sub>CO<sub>3</sub> into a Li<sub>3</sub>PO<sub>4</sub>/MgO composite upon heating. This composite prevents reactions with moisture and CO<sub>2</sub>, ensuring air stability while enhancing Li wettability and reducing interfacial resistance. The Li<sup>+</sup>-conducting Li<sub>3</sub>PO<sub>4</sub> and insulating MgO in the composite interface enable rapid Li<sup>+</sup> diffusion while effectively suppressing electron penetration, resulting in a high critical current density of 1.1 mA·cm<sup>-2</sup>, with stable cycling for over 1200 h at 0.4 mA·cm<sup>-2</sup>. Furthermore, the modified SEs demonstrate excellent cycling stability in Li metal batteries with LiFePO<sub>4</sub> and LiCoO<sub>2</sub> cathodes, confirming the practical feasibility of this solid electrolyte interface modification strategy.