Probing the Air Storage Failure Mechanism of Ni-Rich Layered Cathode Materials

Ni-rich layered oxide cathode materials,such as LiNi_(0.83)Co_(0.12)Mn_(0.05)O_(2)(NCM811),exhibit high specific capacity and low cost,and become cathode material preference of high-energy-density Li-ion batteries.However,these cathode materials are not stable and will form Li-poor reconstructed layers and alkaline compounds(Li_(2)CO_(3),LiOH)on the surface during the storage and processing in humid air,resulting in serious deterioration of electrochemical properties.During the past two decades,the consensus on the surface instability mechanism during humid air storage has not been reached.The main controversy focuses on the unstable octahedron mechanism and the Li/H exchange mechanism.Herein,we investigate the instability mechanism in the humid air by conducting scanning electronic microscopy,scanning transmission electron microscopy,and x-ray photoelectron spectroscopy analysis on NCM811 samples stored in designed atmospheres,etc.,and realize that the surface instability of the NCM811 during storage should be mainly originated from Li/H exchange when it contacts with moisture.

Atomic-resolution characterization on the structure of strontium doped barium titanate nanoparticles

Ferroelectric barium titanate nanoparticles(BTO NPs)may play critical roles in miniaturized passive electronic devices such as multi-layered ceramic capacitors.While increasing experimental and theoretical understandings on the structure of BTO and doped BTO have been developed over the past decade,the majority of the investigation was carried out in thin-film materials;therefore,the doping effect on nanoparticles remains unclear.Especially,doping-induced local composition and structure fluctuation across single nanoparticles have yet to be unveiled.In this work,we use electron microscopy-based techniques including high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM),integrated differential phase contrast(iDPC)-STEM,and energy dispersive X-ray spectroscopy(EDX)mapping to reveal atomically resolved chemical and crystal structure of BTO and strontium doped BTO nanoparticles.Powder X-ray diffraction(PXRD)results indicate that the increasing strontium doping causes a structural transition from tetragonal to cubic phase,but the microscopic data validate substantial compositional and microstructural inhomogeneities in strontium doped BTO nanoparticles.Our work provides new insights into the structure of doped BTO NPs and will facilitate the materials design for next-generation high-density nano-dielectric devices.