Dislocation and oxygen-release driven delithiation in Li₂MnO₃.

ABSTRACT: Lithium-excess layered cathode materials such as Li₂MnO₃ have attracted much attention owing to their high energy densities. It has been proposed that oxygen-release and cation-mixing might be induced by delithiation. However, it is still unclear as to how the delithiated-region grows. Here, by using atomic-resolution scanning transmission electron microscopy combined with electron energy-loss spectroscopy, we directly observe the atomic structures at the interface between pristine and delithiated regions in the partially delithiated Li₂MnO₃ single crystal. We elucidate that the delithiated regions have extensive amounts of irreversible defects such as oxygen-release and Mn/Li cation-mixing. At the interface, a partially cation disordered structure is formed, where Mn migration occurred only in the specific Mn/Li layers. Besides, a number of dislocations are formed at the interface to compensate the lattice mismatch between the pristine and delithiated regions. The observed oxygen-release and dislocations could govern the growth of delithiated-regions and performance degradation in Li₂MnO₃.

SUBMITTER: Nakayama K 

PROVIDER: S-EPMC7479600 | biostudies-literature | 2020 Sep

REPOSITORIES: biostudies-literature