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Given that the performance of a lithium–oxygen battery (LOB) is determined by the electrochemical reactions occurring on the cathode, the development of advanced cathode nanoarchitectures is of great importance for the realization of high‐energy‐density, reversible LOBs. Herein, a robust cathode design is proposed for LOBs based on a dual‐phasic carbon nanoarchitecture. The cathode is composed of an interwoven network of porous metal–organic framework (MOF) derived carbon (MOF‐C) and conductive carbon nanotubes (CNTs). The dual‐phasic nanoarchitecture incorporates the advantages of both components: MOF‐C provides a large surface area for the oxygen reactions and a large pore volume for Li2O2 storage, and CNTs provide facile pathways for electron and O2 transport as well as additional void spaces for Li2O2 accommodation. It is demonstrated that the synergistic nanoarchitecturing of the dual‐phasic MOF‐C/CNT material results in promising electrochemical performance of LOBs, as evidenced by a high discharge capacity of ≈10 050 mAh g−1 and a stable cycling performance over 75 cycles.
A dual‐phasic carbon nanoarchitecture based on an interwoven network of metal–organic framework (MOF) derived carbon (MOF‐C) and carbon nanotubes (CNTs) is proposed as a cathode for rechargeable lithium–oxygen batteries. The synergistic nanoarchitecturing of the high surface area, porous MOF‐C, and conductive CNTs leads to a considerable improvement in the specific capacity, rate‐performance, and cycle lifetime of the batteries.