Monodispersed Ru Nanoparticles Functionalized Graphene Nanosheets as Efficient Cathode Catalysts for O 2 -Assisted Li-CO 2 Battery.

In Li-CO ₂ battery, due to the highly insulating nature of the discharge product of Li ₂ CO ₃ , the battery needs to be charged at a high charge overpotential, leading to severe cathode and electrolyte instability and hence poor battery cycle performance. Developing efficient cathode catalysts to effectively reduce the charge overpotential represents one of key challenges to realize practical Li-CO ₂ batteries. Here, we report the use of monodispersed Ru nanoparticles functionalized graphene nanosheets as cathode catalysts in Li-CO ₂ battery to significantly lower the charge overpotential for the electrochemical decomposition of Li ₂ CO ₃ . In our battery, a low charge voltage of 4.02 V, a high Coulomb efficiency of 89.2%, and a good cycle stability (67 cycles at a 500 mA h/g limited capacity) are achieved. It is also found that O ₂ plays an essential role in the discharge process of the rechargeable Li-CO ₂ battery. Under the pure CO ₂ environment, Li-CO ₂ battery exhibits negligible discharge capacity; however, after introducing 2% O ₂ (volume ratio) into CO ₂ , the O ₂ -assisted Li-CO ₂ battery can deliver a high capacity of 4742 mA h/g. Through an in situ quantitative differential electrochemical mass spectrometry investigation, the final discharge product Li ₂ CO ₃ is proposed to form via the reaction 4Li ⁺ + 2CO ₂ + O ₂ + 4e ^- → 2Li ₂ CO ₃ . Our results validate the essential role of O ₂ and can help deepen the understanding of the discharge and charge reaction mechanisms of the Li-CO ₂ battery.
Competing Interests: The authors declare no competing financial interest.