Tuning the Electronic, Ion Transport, and Stability Properties of Li-rich Manganese-based Oxide Materials with Oxide Perovskite Coatings: A First-Principles Computational Study

(LNMO), a prototypical member of the LRMO family. An accomplished atomistic model is constructed to theoretically estimate the structural, electronic, oxygen vacancy formation energy, and lithium-transport properties of the LNMO/STO interface system, thus providing insightful comparisons with the two integrating bulk materials. It is found that (i) electronic transport in the LNMO cathode is enhanced due to partial closure of the LNMO band gap (∼0.4 eV) and (ii) the lithium ions can easily diffuse near the LNMO/STO interface and within STO due to the small size of the involved ion-hopping energy barriers. Furthermore, the formation energy of oxygen vacancies notably increases close to the LNMO/STO interface, thus indicating a reduction in oxygen loss at the cathode surface and a potential inhibition of undesirable structural phase transitions. This theoretical work therefore opens up new routes for the practical improvement of cost-affordable lithium-rich cathode materials based on highly stable oxide perovskite coatings.