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Although lithium–oxygen batteries have attracted attention due to their extremely high energy densities, rational design, and critical evaluation of high‐energy‐density cathode for practical Li–O2 batteries is still urgently needed. Herein, the multiscale, angstrom‐to‐millimeter, precisely controllable synthesis of binder‐free cathodes with minimally stacked graphene free from edge sites is demonstrated. The proposed Li–O2 battery, based on a hierarchically porous cathode with a practical mass loading of >4.0 mg cm−2, simultaneously exhibits an unprecedented specific areal (>30.0 mAh cm−2), mass (>6300 mAh g−1), and volumetric (>480 mAh cm−3) capacities. The battery displays the optimal energy density of 793 Wh kg−1 critically normalized to the total mass of all active materials including electrolytes and even discharge products Li2O2. Comprehensive in situ characterizations demonstrate a unique discharge mechanism in hierarchical pores which contributes to competitive battery performance. Superior rate performance in a current density range of 0.1 to 0.8 mA cm−2 and long‐cycle stability (>260 cycles) at a current density of 0.4 mA cm−2, outperforming state‐of‐the‐art carbon cathodes. This study yields insight into next‐generation carbon cathodes, not only for use in practical Li–O2 batteries, but also in other metal–gas batteries with high energy densities. [ABSTRACT FROM AUTHOR]

The rational design of a stable and catalytic carbon cathode is crucial for the development of rechargeable lithium‐oxygen (LiO2) batteries. An edge‐site‐free and topological‐defect‐rich graphene‐based material is proposed as a pure carbon cathode that drastically improves LiO2 battery performance, even in the absence of extra catalysts and mediators. The proposed graphene‐based material is synthesized using the advanced template technique coupled with high‐temperature annealing at 1800 °C. The material possesses an edge‐site‐free framework and mesoporosity, which is crucial to achieve excellent electrochemical stability and an ultra‐large capacity (>6700 mAh g−1). Moreover, both experimental and theoretical structural characterization demonstrates the presence of a significant number of topological defects, which are non‐hexagonal carbon rings in the graphene framework. In situ isotopic electrochemical mass spectrometry and theoretical calculations reveal the unique catalysis of topological defects in the formation of amorphous Li2O2, which may be decomposed at low potential (∼ 3.6 V versus Li/Li+) and leads to improved cycle performance. Furthermore, a flexible electrode sheet that excludes organic binders exhibits an extremely long lifetime of up to 307 cycles (>1535 h), in the absence of solid or soluble catalysts. These findings may be used to design robust carbon cathodes for LiO2 batteries. [ABSTRACT FROM AUTHOR]