Promoting the Reversible Oxygen Redox Reaction of Li-Excess Layered Cathode Materials with Surface Vanadium Cation Doping

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Li-excess layered cathode (LLC) materials have a high theoretical specific capacity of 250 mAh g(-1) induced by transition metal (cationic) and oxygen (anionic) redox activity. Especially, the oxygen redox reaction related to the activation of the Li2MnO3 domain plays the crucial role of providing a high specific capacity. However, it also induces an irreversible oxygen release and accelerates the layered-to-spinel phase transformation and capacity fading. Here, it is shown that surface doping of vanadium (V5+) cations into LLC material suppresses both the irreversible oxygen release and undesirable phase transformation, resulting in the improvement of capacity retention. The V-doped LLC shows a high discharge capacity of 244.3 +/- 0.8 mAh g(-1) with 92% retention after 100 cycles, whereas LLC delivers 233.6 +/- 1.1 mAh g(-1) with 74% retention. Furthermore, the average discharge voltage of V-doped LLC drops by only 0.33 V after 100 cycles, while LLC exhibits 0.43 V of average discharge voltage drop. Experimental and theoretical investigations indicate that doped V-doping increase the transition metal-oxygen (TM-O) covalency and affect the oxidation state of peroxo-like (O-2)(n-) species during the delithiation process. The role of V-doping to make the oxygen redox reversible in LLC materials for high-energy density Li-ion batteries is illustrated here.
Publisher
WILEY
Issue Date
2021-03
Language
English
Article Type
Article
Citation

ADVANCED SCIENCE, v.8, no.6

ISSN
2198-3844
DOI
10.1002/advs.202003013
URI
http://hdl.handle.net/10203/285355
Appears in Collection
MS-Journal Papers(저널논문)
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