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Effects of sulfur substitution on chemical bonding nature and electrochemical performance of layered LiMn0.9Cr0.1O2-xSx

Title
Effects of sulfur substitution on chemical bonding nature and electrochemical performance of layered LiMn0.9Cr0.1O2-xSx
Authors
Lim, Seung TaePark, Dae HoonLee, Sun HeeHwang, Seong-JuYoon, Young SooKang, Seong-Gu
Ewha Authors
황성주
SCOPUS Author ID
황성주scopus
Issue Date
2006
Journal Title
BULLETIN OF THE KOREAN CHEMICAL SOCIETY
ISSN
0253-2964JCR Link
Citation
vol. 27, no. 9, pp. 1310 - 1314
Keywords
sulfur substitutionlayered lithium manganatestructural distortioncyclabilityMn migration
Publisher
KOREAN CHEMICAL SOC
Indexed
SCI; SCIE; SCOPUS; KCI WOS scopus
Abstract
Sulfur-substituted LiMn0.9Cro.1O2-xSx (0 <= x <= 0.1) layered oxides have been prepared by solid state reaction under inert atmosphere. From powder X-ray diffraction analyses, all the present lithium manganates were found to be crystallized with monoclinic-layered structure. Electrochemical measurements clearly demonstrated that, in comparison with the pristine LiMn0.9Cr0.1O2, the sulfur-substituted derivatives exhibit smaller discharge capacities for the entire cycle range but the recovery of discharge capacity after the initial several cycles becomes faster upon sulfur substitution. The effect of the sulfur substitution on the chemical bonding nature of LiMn0.9Cr0.1O2-xSx has been investigated using X-ray absorption spectroscopic (XAS) analyses at Mn and Cr K-edges. According to Mn K-edge XAS results, the trivalent oxidation state of manganese ion remains unchanged before and after the substitution whereas the local structure around manganese ions becomes more distorted with increasing the substitution rate of sulfur. On the other hand, the replacement of oxygen with sulfur has negligible influence on the local atomic arrangement around chromium ions, which is surely due to the high octahedral stabilization energy of Cr+III ions. Based on the present experimental findings, we have suggested that the decrease of discharge capacity upon sulfur substitution is ascribable to the enhanced structural distortion of MnO6 octahedra and/or to the formation of covalent Li-S bonds, and the accompanying improvement of cyclability would be related to the depression of Mn migration and/or to the pillaring effect of larger sulfur anion.
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자연과학대학 > 화학·나노과학전공 > Journal papers
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