Li-rich Mn-based layered (LMR) cathodes with anionic redox chemistry show great potential for next-generation sustainable Li-ion battery (LIB) applications due to the low cost and high energy density. However, the asynchronous structural evolutions with cycling in the heterogeneous composite structure of LMR lead to serious lattice strain and thus fast electrochemical decay, which hinders the commercialization of LMR cathodes. Here, an order–disorder coherent LMR cathode is demonstrated that exhibits a higher average voltage (by 0.25 V), negligible voltage decay (97.6% voltage retention after 100 cycles at 100 mA g −1 ), and enhanced cycling stability (98% capacity retention after 200 cycles at 100 mA g −1 ) compared to its layered oxide counterparts. It is proposed that this order–disorder coherent structure design can promote a more synchronous and homogeneous structure evolution during charge and discharge, thus minimizing lattice strain, which significantly prevents layer collapse and collective degradation at high voltage, improving the electrochemical stability. The study displays the feasibility of optimizing the performance of Li-rich cathode materials through a dedicated order–disorder structure control for sustainable energy storage.
All-solid-state batteries (ASSBs) using sulfide electrolytes have attracted ever-increasing interest due to high ionic conductivity of the sulfides. Nevertheless, a thin, strong solid-state sulfide electrolyte membrane maintaining high ionic conductivity is highly desired for ASSBs. Here, a thin, flexible composite solid electrolyte membrane composed of argyrodite sulfide Li 6 PS 5 Cl and a polar poly(vinylidene fluoride- co -trifluoroethylene) (P(VDF-TrFE)) framework is prepared via an electrospinning-infiltration-hot-pressing method. The interaction between Li 6 PS 5 Cl and polar P(VDF-TrFE) ensures a high lithium-ion conductivity (≈1.2 mS cm –1 ) at room temperature and good mechanical ductility of the composite electrolyte membrane. The coin-type ASSB cells with the thin composite electrolyte membrane, a composite cathode of LiNbO 3 -coated LiNi 0.8 Co 0.1 Mn 0.1 O 2 and Li 6 PS 5 Cl, and a lithium-indium anode, show super cycling performance, and the capacity retention is 92% after 1000 cycles and 71% even after 20 000 cycles at 1.0 mA cm –2 (i.e., 1.61 C) at room temperature. Moreover, pouch-type ASSB cells with a high mass loading of active materials are made to demonstrate the potential and feasibility in future commercial applications.
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