Concentration Gradient Induced Delithiation Failure of MoO3 for Li-Ion Batteries
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Abstract
Electric vehicle manufacturers worldwide are demanding superior lithium-ion batteries, with high energy and power densities, compared to gasoline engines. Although conversion-type metal oxides are promising candidates for high-capacity anodes, low initial Coulombic efficiency (ICE) and poor capacity retention have hindered research on their applications. In this study, the ICE of conversion-type MoO3 is investigated, with a particular focus on the delithiation failure. A computational modeling predicts the concentration gradient of Li+ in MoO3 particles. The highly delithiated outer region of the particle forms a layer with low electronic conductivity, which impedes further delithiation. A comparative study using various sizes of MoO3 particles demonstrated that the electrode failure during delithiation is governed by the concentration gradient and the subsequent formation of a resistive shell. The proposed failure mechanism provides critical guidance for the development of conversion-type anode materials with improved electrochemical reversibility.
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