Elsevier

Journal of Power Sources

Volume 68, Issue 2, October 1997, Pages 698-703
Journal of Power Sources

The amorphous oxides MnV2O6 + δ (0 < δ < 1) as high capacity negative electrode materials for lithium batteries

https://doi.org/10.1016/S0378-7753(96)02576-1Get rights and content

Abstract

MnV2O6 + δ · nH2O (0 < δ < 1) amorphous oxides were prepared by a two-step process including the precipitation of a crystallized precursor MnV2O6 · 4H2O and its ozonation at temperatures below 100 °C. Their characterization by spectroscopic techniques (XAS and EELS) shows that V5+ retains a VO5 environment and that Mn, which remains in octahedral coordination, is oxidized to Mn4+ mainly. MnV2O6 + δ compounds insert reversibly large amounts of Li per formula unit (e.g. Li12MnV2O6.96) at low voltage. After the first insertion/de-insertion cycle, subsequent cycles correspond to fully reversible lithium insertion between the two compositions: LiαMnV2O6 + δ (α ≥ 2) and Li12MnV2O6 + δ (from 600 to 900 mAh/g). Investigations on the Li derivatives by XAS and EELS show that during the insertion/de-insertion cycles the V oxidation state varies reversibly between +5 and +3. Mn4+ cations are reduced to Mn2+ upon the first discharge. During the subsequent cycles the average Mn oxidation state varies reversibly between +2 and about +2.6. It clearly appears that the electron transfer from Li to the host matrix decreases with increasing x in LixMnV2O6 + δ.

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    The platform indicates that the chemical and structural changed correspond to a series of phase transitions occurring when Li+ embed in V6O13 [22,23]. Among them, the discharge platform at 2.6 V corresponds to the variation of V5+ to V4+ [24], and 2.2 V corresponded to the variation of V4+ to V3+ [25]. The first discharge platform increases first and decreases later with the increase of the doped amounts, which also correspond to the discharge capacity curves.

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Present address: Department of chemistry, University of Waterloo, 200 University Ave. W., Waterloo, Ontario N2L 3G1, Canada.

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