Furthermore, we have recently provided a novel strategy to suppress Mn dissolution and the JT distortion by investigating the spinel LMO (001) surface with a single layer of graphene using DFT.2 Our theoretical calculation in Ref. 2 suggests that the interaction between the graphene sheet and the LMO (001) surface suppresses the Mn3+ disproportionation reaction into Mn2+ and Mn4+. While all surface Mn atoms at the LMO (001) have an oxidation state of +3, we find that the (001) Mn atom that chemically bonds with graphene adopts an electron configuration that has a clear +4 character with an empty eg band. By analyzing the (001) LMO surface Mn-O bond distance, we observe that the JT distortion is reduced as the oxidation state of surface Mn shifts to Mn4+ in the presence of the graphene sheet. A chemical bonding between graphene and LMO on the (001) surfaces provides an underlying mechanism that electronically modifies the LMO (001) surfaces, and subsequently stabilizes them against Mn3+ disproportionation reaction and the JT distortion by converting (001) surface Mn3+ to Mn4+. Our advanced first-principles computations shed lights on the development of alternative hybrid Mn-cathode architecture approaches that can overcome the key shortcomings in these cathode materials.
 S. Kim, M. Aykol, and C. Wolverton. Phys. Rev. B, 92, 115411.
 L. Jaber-Ansari, K. P. Puntambekar, S. Kim, M. Aykol, L. Luo, J. Wu, B. D. Myers, H. Iddir, J. T. Russell, S. J. Saldaña, R. Kumar, M. M. Thackeray, L. A. Curtiss, V. P. Dravid, C. Wolverton, and M. C. Hersam. Adv. Energy. Mater. 5 (2015) 1500646
This computational research work was supported by Northwestern-Argonne Institute of Science and Engineering (NAISE) and the Dow Chemical Company.