Exploring the Cathode Active Materials for Sulfide‐Based All‐Solid‐State Lithium Batteries with High Energy Density

• Published in: Small (Weinheim an der Bergstrasse, Germany) Germany), 2024-03, Vol.20 (9), p.e2304747-n/a
• Main Authors: Hong, Seung‐Bo, Lee, Young‐Jun, Lee, Han‐Jo, Sim, Hui‐Tae, Lee, Hyobin, Lee, Yong Min, Kim, Dong‐Won
• Format: Article
• Language: English
• Subjects: all‐solid‐state batteries; cathode active materials; Cathodes; digital‐twin modeling; Electrolytes; High temperature; Ion currents; Lithium; Lithium batteries; Lithium-ion batteries; Molten salt electrolytes; nickel‐rich cathodes; Particle size; Solid electrolytes; sulfide solid electrolytes
• ISSN: 1613-6810; 1613-6829
• DOI: 10.1002/smll.202304747

All‐solid‐state lithium batteries (ASSLBs) are considered promising alternatives to current lithium‐ion batteries that employ liquid electrolytes due to their high energy density and enhanced safety. Among various types of solid electrolytes, sulfide‐based electrolytes are being actively studied, because they exhibit high ionic conductivity and high ductility, which enable good interfacial contacts in solid electrolytes without sintering at high temperatures. To improve the energy density of the sulfide‐based ASSLBs, it is essential to increase the loading of active material in the composite cathode. In this study, the Ni‐rich LiNixCoyMn1‐x‐yO2 (NCM) materials are explored with different Ni content, particle size, and crystalline form to probe suitable cathode active materials for high‐performance ASSLBs with high energy density. The results reveal that single‐crystalline LiNi0.82Co0.10Mn0.08O2 material with a small particle size exhibits the best cycling performance in the ASSLB assembled with a high mass loaded cathode (active mass loading: 26 mg cm−2, areal capacity: 5.0 mAh cm−2) in terms of discharge capacity, capacity retention, and rate capability. Single‐crystalline LiNi0.82Co0.10Mn0.08O2 material with a small particle size exhibits the best cycling performance in the all‐solid‐state lithium batteries (ASSLBs) assembled with a high mass loaded cathode (active mass loading: 26 mg cm−2, areal capacity: 5.0 mAh cm−2) in terms of discharge capacity, capacity retention, and rate capability. The results reveal conclusive guidance for selecting suitable cathode active material for ASSLBs.