Pseudo-trilayer Organoclay Enables Directed Li⁺ Transport and Anion Trapping in Quasi-Solid-State Gel Electrolytes

Enhancing Li⁺ transport while ensuring safety is crucial for the development of high-energy density batteries. While nanomaterials boost ionic conductivity in quasi-solid state gel electrolyte (QSE), the transport mechanisms remain unclear. This study presents a synthetic strategy utilizing tailored two-dimensional saponite clay additives with a controlled organic cation configuration to achieve superior Li-ion conductivity in QSE. This optimized configuration enables rapid, uniform Li⁺ movement through controlled interlayers and effective anion trapping within aligned surfactant domains. Consequently, a pseudo-trilayer configuration of organoclay serves as a fast Li⁺ transport pathway in the QSE, leading to a high Li⁺ transference number of 0.71 and stable cycling performance for 1000 h. Moreover, batteries utilizing the pseudo-trilayer organoclay demonstrate compatibility with the LiNi_0.9Mn_0.05Co_0.05O₂ cathode, maintaining 86.7% capacity retention after 200 cycles. This work suggests a design strategy for advanced QSE that precisely controls the Li⁺ transport route, contributing to a high energy density with minimal additives.