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Li-air batteries (LABs) are promising because of their high energy density. However, LABs are troubled by large electrochemical polarization during discharge and charge, side reactions from both carbon cathode surface/peroxide product and electrolyte/superoxide intermediate, as well as the requirement for pure O 2 . Here we report the solution using multiwall carbon nanotubes (MCNTs)@MnO 2 nanocomposite cathode integrated with N,N'-bis(salicylidene)ethylenediaminocobalt(II) (Co II -salen) in electrolyte for LABs. The advantage of such a combination is that on one hand, the coating layer of δ-MnO 2 with about 2-3 nm on MCNTs@MnO 2 nanocomposite catalyzes Li 2 O 2 decomposition during charge and suppresses side reactions between product Li 2 O 2 and MCNT surface. On the other hand, Co II -salen works as a mobile O 2 -carrier and accelerates Li 2 O 2 formation through the reaciton of (Co III -salen) 2 -O 2  2- + 2Li + + 2e - → 2Co II -salen + Li 2 O 2 . This reaction route overcomes the pure O 2 limitation and avoids the formation of aggressive superoxide intermediate (O 2  - or LiO 2 ), which easily attacks organic electrolyte. By using this double-catalyst system of Co-salen/MCNTs@MnO 2 , the lifetime of LABs is prolonged to 300 cycles at 500 mA g -1 (0.15 mA cm -2 ) with fixed capacity of 1000 mAh g -1 (0.30 mAh cm -2 ) in dry air (21% O 2 ). Furthermore, we up-scale the capacity to 500 mAh (5.2 mAh cm -2 ) in pouch-type batteries (∼4 g, 325 Wh kg -1 ). This study should pave a new way for the design and construction of practical LABs.

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MCNTs@MnO<sub>2</sub> Nanocomposite Cathode Integrated with Soluble O<sub>2</sub>-Carrier Co-salen in Electrolyte for High-Performance Li–Air Batteries

MCNTs@MnO2 Nanocomposite Cathode Integrated with Soluble O2-Carrier Co-salen in Electrolyte for High-Performance Li–Air Batteries

MCNTs@MnO₂ Nanocomposite Cathode Integrated with Soluble O₂-Carrier Co-salen in Electrolyte for High-Performance Li–Air Batteries