Li7La3Zr2O12-co-LiNbO3 Surface Modification Improves the Interface Stability between Cathode and Sulfide Solid-State Electrolyte in All-Solid-State Batteries.

With the rapid development of energy storage and electric vehicles, thiophosphate-based all-solid-state batteries (ASSBs) are considered the most promising power source. In order to commercialize ASSBs, the interfacial problem between high-voltage cathode active materials and thiophosphate-based solid-state electrolytes needs to be solved in a simple, effective way. Surface coatings are considered the most promising approach to solving the interfacial problem because surface coatings could prevent direct physical contact between cathode active materials and thiophosphate-based solid-state electrolytes. In this work, Li7La3Zr2O12 (LLZO) and LiNbO3 (LNO) coatings for LiCoO2 (LCO) were fabricated by in-situ interfacial growth of two high-Li+ conductive oxide electrolytes on the LCO surface and tested for thiophosphate-based ASSBs. The coatings were obtained from a two-step traditional sol-gel coatings process, the inner coatings were LNO, and the surface coatings were LLZO. Electrochemical evaluations confirmed that the two-layer coatings are beneficial for ASSBs. ASSBs containing LLZO-co-LNO coatings LiCoO2 (LLZO&LNO@LCO) significantly improved long-term cycling performance and discharge capacity compared with those assembled from uncoated LCO. LLZO&LNO@LCO||Li6PS5Cl (LPSC)||Li-In delivered discharge capacities of 138.8 mAh/g, 101.8 mAh/g, 60.2 mAh/g, and 40.2 mAh/g at 0.05 C, 0.1 C, 0.2 C, and 0.5 C under room temperature, respectively, and better capacity retentions of 98% after 300 cycles at 0.05 C. The results highlighted promising low-cost and scalable cathode material coatings for ASSBs.

Nonporous Gel Electrolytes Enable Long Cycling at High Current Density for Lithium-Metal Anodes.

Lithium-metal anodes with high theoretical capacity and ultralow redox potential are regarded as a "holy grail" of the next-generation energy-storage industry. Nevertheless, Li inevitably reacts with conventional liquid electrolytes, resulting in uneven electrodeposition, unstable solid electrolyte interphase, and Li dendrite formation that all together lead to a decrease in active lithium, poor battery performance, and catastrophic safety hazards. Here, we report a unique nonporous gel polymer electrolyte (NP-GPE) with a uniform and dense structure, exhibiting an excellent combination of mechanical strength, thermal stability, and high ionic conductivity. The nonporous structure contributed to a uniform distribution of lithium ions for dendrite-free lithium deposition, and Li/NP-GPE/Li symmetric cells can maintain an extremely low and stable polarization after cycling at a high current density of 10 mA cm-2. This work provides an insight that the NP-GPE can be considered as a candidate for practical applications for lithium-metal anodes.