![]() One that stands out and has been proven to be an effective coating material is LiNbO 3 (apparently because of favorable charge-transport properties in the amorphous state) 36. Hence, in order to achieve stable cycling of the cathode, the outer surface of the storage particles needs to be covered by a protective layer 28, 29, 30, with Li-based oxides being the most widely studied coating materials (e.g., LiNbO 3 31, LiTaO 3 32, Li 2ZrO 3 33, Li 4Ti 5O 12 34 or Li 2CO 3 35). However, combining such cathode materials with lithium thiophosphate solid electrolytes is hampered by side reactions at the interfaces during electrochemical cycling, leading to low reversibility and impedance buildup and therefore to performance decay 22, 23, 24, 25, 26, 27. At the positive electrode side, Ni-rich layered lithium metal oxides, such as LiNi 1– x– 圜o xMn yO 2 (NCM or NMC) or LiNi 1– x– zCo xAl zO 2 (NCA) with ≥ 0.6 Ni content, are regarded generally as state-of-the-art cathode materials for bulk solid-state battery (SSB) applications 18, 19, 20, 21, as in the case of energy-dense LIBs. Lithium thiophosphates, such as argyrodite Li 6PS 5Cl, are among the most promising solid electrolytes because of their high ionic conductivity at room temperature and favorable ductility properties 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17. Substituting an inorganic (superionic) solid electrolyte for the liquid electrolyte in LIBs is a potentially viable strategy to increase energy density and minimize safety risks due to cell failure 4, 5, 6. The demand for energy storage is growing strongly, largely driven by the automotive industry. Li-ion batteries (LIBs) using liquid organic electrolytes play a pivotal role in our modern society, especially for powering portable electronic devices and electric vehicles 1, 2, 3. Our research data indicate that a hybrid coating may in fact be beneficial to the kinetics and the cycling performance strongly depends on the solid electrolyte used. In the present work, we examine how surface carbonates incorporated into the sol–gel-derived LiNbO 3 protective coating on NCM622 cathode material affect the efficiency and rate capability of pellet-stack solid-state battery cells with β-Li 3PS 4 or argyrodite Li 6PS 5Cl solid electrolyte and a Li 4Ti 5O 12 anode. Hence, effective surface coatings are required to mitigate or ideally prevent detrimental reactions from occurring and having an impact on the cyclability. However, interfacial side reactions between the individual components during battery operation usually result in accelerated performance degradation. In particular, layered lithium metal oxides and lithium thiophosphates hold promise as cathode materials and superionic solid electrolytes, respectively. While still premature as an energy storage technology, bulk solid-state batteries are attracting much attention in the academic and industrial communities lately.
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