Regulating the Manganese Valence State Improves the Kinetic Properties of Manganese‐Based Cathodes

Abstract Manganese (Mn)‐based lithium (Li)‐ion batteries with high energy density and low cost have recently attracted considerable attention. One drawback of Mn‐based batteries is the severe capacity attenuation caused by the Jahn‐Teller effect, which distorts the crystal structure and reduces the kinetics of Li‐ion insertion/extraction in the cathodes. In this study, the Mn valence state is regulated on the surface of Mn‐based oxide particles and oxygen vacancies are introduced to facilitate rapid Li‐ion transport and charge storage by adding succinonitrile (SN) to Mn‐based cathodes. Because of the reaction between SN and Mn‐based cathode particles, the contents of Mn 3+ ions and oxygen vacancies increase, leading to an improvement in the Li‐ion kinetic properties of the cathodes as well as a reduction in the dissolution of Mn from the cathodes. By regulating the Mn valence state, Li‐ion and Li metal batteries with LiMn 2 O 4 or Li‐rich Mn‐based layered oxide cathodes show significantly enhanced discharge capacity and improved cyclic performance. This study demonstrates that regulating the valence state of Mn ions is an effective strategy for enhancing the electrochemical performance of Mn‐based Li batteries and that adding SN to the cathodes is a cost‐effective method for mass production.