First Principles Investigation of Stable LiMn2O4 Surfaces for Lithium-Ion Batteries
In this work, we investigate the effects of surface termination, slab reconstruction, relaxation schemes, magnetic ordering, and different U value for Mn to determine the relative stabilities of the LMO surfaces. We find that it is necessary to relax all atomic positions with symmetry-broken DFT calculations to fully capture the local variation of Mn-O and Li-O polyhedral clusters to obtain the most consistent surface energies. We finally comment on the possible implication of our work on the future surface studies of the mixed-valence transition metal complex oxides such as the LMO system.
Acknowledgement: This work has been supported by Northwestern-Argonne Institute of Science and Engineering (NAISE) and by The Dow Chemical Company.