RuO₂-Incorporated Co₃O₄ Nanoneedles Grown on Carbon Cloth as Binder-Free Integrated Cathodes for Tuning Favorable Li₂O₂ Formation

Developing ideal Li–O2 batteries (LOBs) requires the discharge product to have a large quantity, have large contact area with the cathode, and not passivate the porous surface after discharge, which put forward high requirement for the design of cathodes. Herein, combining the rational structural design and high activity catalyst selection, minor amounts of RuO2-incorporated Co3O4 nanoneedles grown on carbon cloth are successfully synthesized as binder-free integrated cathodes for LOBs. With this unique design, plenty of electron–ion–oxygen tri-phase reaction interface is created, the side reaction from carbon is isolated, and oxygen reduction reaction/oxygen evolution reaction (OER) kinetics are significantly facilitated. Upon discharge, film-like Li2O2 is observed growing on the needle surface first and eventually ball-like Li2O2 particles form at each tip of the needle. The cathode surface remains porous after discharge, which is beneficial to the OER and is rare in the previous reports. The battery exhibits a high specific discharge capacity (7.64 mAh cm–2) and a long lifespan (500 h at 0.1 mA cm–2). Even with a high current of 0.3 mA cm–2, the battery achieves a cycling life of 200 h. In addition, punch-type LOBs are fabricated and successfully operated, suggesting that the cathode material can be utilized in ultralight, flexible electronic devices.