Dandelion-like Mn/Ni Co-doped CoO/C Hollow Microspheres with Oxygen Vacancies for Advanced Lithium Storage.

Abstract

Hollow structures have attracted great attention based on the advantage to accommodate volume expansion. However, template removal usually results in structure destruction. Herein, dandelion-like Mn/Ni co-doped CoO/C hollow microspheres (CMNC-10h) are synthesized via an Ostwald ripening process without templates. The high-angle annular dark field mapping images at the atomic level indicate the successful doping of Mn and Ni into CoO. Via an annular bright field image, oxygen vacancies induced by doping can be clearly observed. The residual two electrons in the oxygen vacancy site are highly delocalized, as confirmed by density functional theory calculations, effectively improving electrical conductivity. According to electron holography analysis, the dielectric polarization field in superficial regions of primary nanoparticles can facilitate insertion of Li+ ions into nanoparticles and thus enhance electrochemical kinetics. Combining those advantages, CMNC-10h demonstrates a high capacity of 1126 mAh g-1 at 1 A g-1 after 1000 cycles as anode material for a lithium-ion battery. Additionally, based on the strong adsorption toward polysulfide, the porous structure to accommodate sulfer/polysulfide, and the effects of oxygen vacancies to immobilize and catalyze polysulfide, CMNC-10h-S as cathode material for a lithium-sulfur battery also displays a high capacity of 642 mAh g-1 after 500 cycles at 1 C.