Assessing the Performance of Cobalt Phthalocyanine Nanoflakes as Molecular Catalysts for Li-Promoted Oxalate Formation in Li–CO2–Oxalate Batteries

Removal of O2 molecules from the cathode environment in the Li-based battery has led to introduction of the Li–CO2 battery as the novel and promising source of energy storage. In spite of CO2 capture through the reversible reaction between Li atoms and CO2 molecules at the cathode, the performance of the Li–CO2 battery is hampered by formation of the Li2CO3 insulating product in the discharge process and its difficult decomposition in the charging process. Hereby, we explore the possible improvement of the performance of the Li–CO2 battery through replacement of Li2CO3 by Li2C2O4 as the discharge product. This is achieved by systematic addition of Li and CO2 to a cobalt phthalocyanine (CoPc) nanoflake employed as the molecular catalyst in the cathode of the Li–CO2 battery by means of computational density functional theory-based methods. The present results predict high adsorption energy of the CO2 molecules (−2.16 eV), low Li-intercalation voltage (1.45 V), reveal the important and constructive influence...