Rechargeable lithium-ion batteries that use an aqueous electrolyte have been developed. Cells with LiMn(2)O(4) and VO(2)(B) as electrodes and 5 M LiNO(3) in water as the electrolyte provide a fundamentally safe and cost-effective technology that can compete with nickelcadmium and lead-acid batteries on the basis of stored energy per unit of weight.
LiNixMn2−xO4
has been synthesized using sol‐gel and solid‐state methods for 0 < x < 0.5. The electrochemical behavior of the samples was studied in
normalLi/LiNixMn2−xO4
coin‐type cells. When x = 0, the capacity of
normalLi/LiMn2O4
cells appears at 4.1 V. As x increases, the capacity of the 4.1 V plateau decreases as 1−2x Li per formula unit, and a new plateau at 4.7 V appears. The capacity of the 4.7 V plateau increases as 2x Li per formula unit, so that the total capacity of the samples (both the 4.1 and 4.7 V plateaus) is constant. This is taken as evidence that the oxidation state of Ni in these samples is +2, and therefore they can be written as
Li+1Nix+2Mn1−2x+3Mn1+x+4O4−2
. The 4.1 V plateau is related to the oxidation of
Mn3+
to
Mn4+
and the 4.7 V plateau to the oxidation of
Ni2+
to
Ni4+
. The effect of synthesis temperature, atmosphere, and cooling rate on the structure and electrochemical properties of
LiNi0.5Mn1.5O4
is also studied on samples made by the sol‐gel method.
LiNi0.5Mn1.5O4
samples made by heating gels at temperatures below 600°C in air are generally oxygen deficient, leading to Mn oxidation states significantly less than 4.
LiNi0.5Mn1.5O4
samples heated above 650°C suffer due to disproportionation into
LiNixMn2−xO4
with x < 0.5 and
LizNi1−zO
with z ≈ 0.2, which occurs above about 650°C. Pure
LiNi0.5Mn1.5O4
materials can be made by extended heatings near 600°C or by slowly cooling materials heated at higher temperatures.
LiNi0.5Mn1.5O4
made at 600°C has demonstrated good reversible capacity at 4.7 V in excess of 100 mAh/g for tens of cycles.
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