Role of Superexchange Interactions on the Arrangement of Fe and Mn in LiMnxFe1–xPO4

Due to excellent safety and charge–discharge performances of LiFePO4 (LFP), it has been widely studied as an important cathode material for lithium-ion batteries. The introduction of Mn ions to LFP materials to increase the voltage and energy storage is a hot topic that has attracted widespread attention. Our study focused on calculating the transition metal (TM) ion arrangement in LiMn1–xFexPO4 (LMFP). Superexchange interactions were observed to affect the TM structure sequence and magnetic structure in LMFP, indicating that Mn ions tend to have a specific clustering arrangement in the TM layer that is bridged by shared O ions. The overall magnetic structure is antiferromagnetic.