Chemistry of Materials
Chemistry of Materials
5 years ago

Surface Reconstruction in Li-Rich Layered Oxides of Li-Ion Batteries

Surface Reconstruction in Li-Rich Layered Oxides of Li-Ion Batteries
Raymond R. Unocic, Paulo J. Ferreira, Arumugam Manthiram, Karalee Jarvis, Maria Varela, Chih-Chieh Wang
The performance characteristics of lithium-ion battery cathode materials are governed by the surface structure and chemistry. Synthesis is known to affect the structure of these materials; however, a full understanding of the effects of the surface structure is not well understood. Here, we explore the atomic scale structure of lithium-layered oxides prepared with two different thermal treatments. We show that, under certain thermal treatments, the surface perpendicular to the transition-metal layers is enriched in nickel, which results in Ni occupying the lithium layer of the layered oxide structure. Under both thermal treatments, this surface also shows a reduction of Mn, with some of the reduced Mn occupying sites in the lithium layer. The surface parallel to the transition-metal layers under both treatments shows significant Mn reduction, oxygen loss, and reduced Mn in the lithium layer. The Mn reduction and surface reconstruction are the result of unstable surface terminations and are intrinsic to layered oxides. Synthesis can be tuned to eliminate Ni enrichment at the surface; however, it cannot be tailored to eliminate Mn reduction and surface reconstruction.

Publisher URL: http://dx.doi.org/10.1021/acs.chemmater.7b00120

DOI: 10.1021/acs.chemmater.7b00120

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