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 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.