can provide a promising strategy for green usage of CO 2 from the atmosphere. [6][7][8][9] The concept of aprotic lithium-CO 2 battery is proposed, in which the mechanism is based on the electrochemical reaction, 4Li + + 3CO 2 + 4e -<=> 2Li 2 CO 3 + C (E o = 2.80 V vs Li/Li + ), composed of CO 2breathing electrode as cathodes, lithium metal as anodes, and lithium salt dissolved in aprotic solvent as electrolyte. [6,9,10] Although the specific pathway of CO 2 reduction reaction is still unclear, it is generally accepted that the reduction reaction proceeds through the general steps shown below [8,9,11,12] ) has been proved to form on the electrode at the beginning of discharge process by the in situ surface-enhanced Raman spectroscopy. [11] And the mechanism of the electroreduction of CO 2 in aprotic solvents has also been reported, in which the CO 2 is reduced to CO 2 by one-electron reaction, Aprotic Li-CO 2 batteries are a new class of green energy storage and conversion system, which can utilize the CO 2 from the atmosphere in an environmentally friendly way. However, the biggest problem of the existing Li-CO 2 batteries is that they suffer from high polarization and poor cycling performance, mainly caused by the insulating and insoluble discharge product, Li 2 CO 3 . Herein, this study reports the synthesis of wrinkled, ultrathin Ir nanosheets fully anchored on the surface of N-doped carbon nanofibers (Ir NSs-CNFs) as an efficient cathode for improving the performance of lithium-CO 2 batteries. The battery can be steadily discharged and charged at least for 400 cycles with a cut-off capacity of 1000 mAh g −1 at 500 mA g −1 . Meanwhile, the cathode can effectively reduce the charge overpotential by showing a charge termination voltage below 3.8 V at 100 mA g −1 , which is the smallest charge overpotential reported to date. The ex situ analysis of the intermediate products reveals that during the discharge process, Ir NSs-CNFs can greatly stabilize amorphous granular intermediate (probably Li 2 C 2 O 4 ) and delay its further transformation into thin plate-like Li 2 CO 3 , whereas during the charge process, it can make Li 2 CO 3 be easily and completely decomposed, which is the key in greatly improving its performance for lithium-CO 2 batteries.
Lithium-CO 2 BatteriesThe energy shortage and environmental pollution are the severe challenges for achieving the sustainable development of the human society. [1,2] Unfortunately, the main energy resources in the present society are still fossil fuels, which undoubtedly are nonrenewable, and produce a mass of greenhouse gases, resulting in accelerating the global temperature rise. [3][4][5] How to capture and convert CO 2 into renewable energy in an environmentally friendly way is attracting more intensive attention.Recently, the lithium-CO 2 battery as an innovative energy storageThe ORCID identification number(s) for the author(s) of this article can be found under https://doi.