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Free, publicly-accessible full text available January 1, 2025
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Xiao, Yihan ; Jun, KyuJung ; Wang, Yan ; Miara, Lincoln J. ; Tu, Qingsong ; Ceder, Gerbrand ( , Advanced Energy Materials)
Abstract The key component in lithium solid‐state batteries (SSBs) is the solid electrolyte composed of lithium superionic conductors (SICs). Lithium oxide SICs offer improved electrochemical and chemical stability compared with sulfides, and their recent advancements have largely been achieved using materials in the garnet‐ and NASICON (sodium superionic conductor)‐ structured families. In this work, using the ion‐conduction mechanisms in garnet and NASICON as inspiration, a common pattern of an “activated diffusion network” and three structural features that are beneficial for superionic conduction: a 3D percolation Li diffusion network, short distances between occupied Li sites, and the “homogeneity” of the transport path are identified. A high‐throughput computational screening is performed to search for new lithium oxide SICs that share these features. From this search, seven candidates are proposed exhibiting high room‐temperature ionic conductivity evaluated using ab initio molecular dynamics simulations. Their structural frameworks including spinel, oxy‐argyrodite, sodalite, and LiM(SeO3)2present new opportunities for enriching the structural families of lithium oxide SICs.
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Zhang, Ya‐Qian ; Tian, Yaosen ; Xiao, Yihan ; Miara, Lincoln J. ; Aihara, Yuichi ; Tsujimura, Tomoyuki ; Shi, Tan ; Scott, M. C. ; Ceder, Gerbrand ( , Advanced Energy Materials)
Abstract The interfacial instability between a thiophosphate solid electrolyte and oxide cathodes results in rapid capacity fade and has driven the need for cathode coatings. In this work, the stability, evolution, and performance of uncoated, Li2ZrO3‐coated, and Li3B11O18‐coated LiNi0.5Co0.2Mn0.3O2cathodes are compared using first‐principles computations and electron microscopy characterization. Li3B11O18is identified as a superior coating that exhibits excellent oxidation/chemical stability, leading to substantially improved performance over cells with Li2ZrO3‐coated or uncoated cathodes. The chemical and structural origin of the different performance is interpreted using different microscopy techniques which enable the direct observation of the phase decomposition of the Li2ZrO3coating. It is observed that Li is already extracted from the Li2ZrO3in the first charge, leading to the formation of ZrO2nanocrystallites with loss of protection of the cathode. After 50 cycles separated (Co, Ni)‐sulfides and Mn‐sulfides can be observed within the Li2ZrO3‐coated material. This work illustrates the severity of the interfacial reactions between a thiophosphate electrolyte and oxide cathode and shows the importance of using coating materials that are absolutely stable at high voltage.