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Fully Reversible Homogeneous and Heterogeneous Li Storage in RuO2 with High Capacity

In this paper, we report that Li can be stored in RuO2 with an unusually high coulombic efficiency. The process involves three electrochemical steps: i) formation of a Ru/Li2O nanocomposite, ii) formation of a Li‐containing surface film, and iii) interfacial deposition of Li within the Ru/Li2O matrix. Corresponding to the storage of 5.6 mole of Li ions per mole of RuO2, a high capacity of 1130 mAh g–1 is achieved. Furthermore, virtually all inserted Li ions can be extracted, corresponding to a nearly 100 % coulombic efficiency at the first cycle. Achieving a complete reversibility for such a Li storage system through complex heterogeneous solid‐state electrochemical reactions is possible because of the formation of nanoscale Ru/Li2O during Li insertion and nano‐RuO2 during Li extraction, in addition to the favorable transport properties of RuO2 itself.