Highly Rechargeable Lithium‐CO₂ Batteries with a Boron‐ and Nitrogen‐Codoped Holey‐Graphene Cathode

Metal‐air batteries, especially Li‐air batteries, have attracted significant research attention in the past decade. However, the electrochemical reactions between CO 2 (0.04 % in ambient air) with Li anode may lead to the irreversible formation of insulating Li 2 CO 3 , making the battery less rechargeable. To make the Li‐CO 2 batteries usable under ambient conditions, it is critical to develop highly efficient catalysts for the CO 2 reduction and evolution reactions and investigate the electrochemical behavior of Li‐CO 2 batteries. Here, we demonstrate a rechargeable Li‐CO 2 battery with a high reversibility by using B,N‐codoped holey graphene as a highly efficient catalyst for CO 2 reduction and evolution reactions. Benefiting from the unique porous holey nanostructure and high catalytic activity of the cathode, the as‐prepared Li‐CO 2 batteries exhibit high reversibility, low polarization, excellent rate performance, and superior long‐term cycling stability over 200 cycles at a high current density of 1.0 A g −1 . Our results open up new possibilities for the development of long‐term Li‐air batteries reusable under ambient conditions, and the utilization and storage of CO 2 .