Intelligently tuning the electronic structure of solid catalyst for bidirectional electrode process in lithium-oxygen batteries

In lithium-oxygen (Li-O2) batteries, catalytic conversion of lithium superoxide (LiO2) is a critical step to enhance kinetics. However, it is challenging for catalysts to be both highly efficient in the charging and discharging processes owing to the varying electrochemical en-vironments. Here, we have achieved the desirable catalysis for the bidirectional electrode process by intelligently tuning the electronic structure of platinum/vanadium oxide (Pt/VOx). Due to changes in the internal electric field, the structure of Pt/VOx dynamically evolves during cycling (Pt/V2O3 or Pt/V2O5). The different redox states of the VOx can dynamically tune the electron density of Pt due to the strong metal-support interaction (SMSI), resulting in desirable adsorption behavior for LiO2 in the bidirectional electrode process. Consequently, Li-O2 batteries with Pt/VOx electrodes show ultra-low charge overpotential (0.14 V) and higher capacity (13,270 mAh g-1), indicating the great potential of catalyst recon-struction for high-performance Li-O2 batteries.