Abstract
Ion exchange reactions and Li insertion in the (M is transition metal and ) hollandite‐type structure compounds have been investigated. Several new phases were synthesized at 450°C by an ion exchange reaction using alkali halide salts. A correlation between the ionicity of the M‒O bonds and conductivity was confirmed, but no samples exhibited an ionic conductivity exceeding 10−4 Ω−1 cm−1 at 200°C. For the first time it was shown that Li can be chemically or electrochemically intercalated into hollandite‐type phases as with ranging from 0 to 6. Electrochemical and in situ x‐ray powder diffraction measurements have shown that Li insertion in these compounds proceeds at voltages lower than 1.2V and is partially reversible. Upon lithiation, the material undergoes a reversible phase transition. Because of their low Li intercalation voltages, these materials could possibly be used as anodes, instead of Li metal, in secondary Li cells.
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