Abstract
Oxygen release is a major issue associated with layer-structured metal oxide cathodes in lithium batteries, which can further cause a series of problems, such as irreversible phase transition, microcracking, and electrolyte decomposition. Eventually, these issues jointly result in cell performance degradation and safety hazards. Thus, it is very significant to tackle oxygen release for achieving long-term stable cyclability, but very challenging. Although intensive efforts have been invested to date, there still lacks a feasible solution. In this study, nanoscale ZrS(2) coatings are applied on prefabricated LiNi(0.8)Mn(0.1)Co(0.1)O(2) (NMC811) cathodes directly via atomic layer deposition (ALD). Very encouragingly, we reveal that this ALD-deposited conformal ZrS(2) nanocoating can serve as an exceptional oxygen scavenger and then convert into a stable sulfate (Zr(SO(4))(2)) coating. Such an in situ conversion is very beneficial and effective for protecting the electrolyte from decomposition. In addition, the resultant Zr(SO(4))(2) coating further inhibits undesirable reactions, stabilizes the interface between NMC811 and the electrolyte, suppresses microcracking, mitigates transition metal dissolution, and maintains the structural stability of the NMC811 cathode. Consequently, the ZrS(2)-coated NMC811 cathode has demonstrated extraordinary performance. Thus, this study advances the understanding of interface engineering while paving a new technical pathway for commercializing NMC811 cathodes.