Tuning the Covalent Coupling Degree between the Cathode and Electrolyte for Optimized Interfacial Resistance in Solid-State Lithium Batteries

The development of promising solid-state lithium batteries has been a challenging task mainly due to the poor interfacial contact and high interfacial resistance at the electrode/solid-state electrolyte (SSE) interface. Herein, we propose a strategy for introducing a class of covalent interactions with varying covalent coupling degrees at the cathode/SSE interface. This method significantly reduces interfacial impedances by strengthening the interactions between the cathode and SSE. By adjusting the covalent coupling degree from low to high, an optimal interfacial impedance of 33 Ω cm–2 was achieved, which is even lower than the interfacial impedance using liquid electrolytes (39 Ω cm–2). This work offers a fresh perspective on solving the interfacial contact problem in solid-state lithium batteries.