Metal‐air batteries, especially Li‐air batteries, have attracted significant research attention in the past decade. However, the electrochemical reactions between CO2 (0.04 % in ambient air) with Li anode may lead to the irreversible formation of insulating Li2CO3, making the battery less rechargeable. To make the Li‐CO2 batteries usable under ambient conditions, it is critical to develop highly efficient catalysts for the CO2 reduction and evolution reactions and investigate the electrochemical behavior of Li‐CO2 batteries. Here, we demonstrate a rechargeable Li‐CO2 battery with a high reversibility by using B,N‐codoped holey graphene as a highly efficient catalyst for CO2 reduction and evolution reactions. Benefiting from the unique porous holey nanostructure and high catalytic activity of the cathode, the as‐prepared Li‐CO2 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 CO2.
A lithium-CO2 battery with a holey graphene catalyst exhibited high rechargeability and superior long-term cycling stability over 200 cycles at ambient temperature. Previously, the electrochemical reaction between CO2 with the Lithium anode led to formation of insulating Li2CO3, making the battery less rechargeable.