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It is generally understood that particle‐shaped Li2O2 is preferred in Li‐O2 batteries (LOBs) because the dominance of Li2O2 films may lead to poor electrochemical performance. The influence of Li2O2 morphology and its nucleation mechanism are probed by experiments along with the first‐principle calculations. It is revealed that the LOBs with Li2O2 films deliver unexpectedly improved capacities, longer...
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