Electron structure and reaction pathway regulation on porous cobalt-doped CeO2/graphene aerogel: A free-standing cathode for flexible and advanced Li-CO2 batteries

Li-CO 2 batteries present considerable prospects both in resourcing CO 2 and remedying the unsatisfied performance of current energy storage devices. Herein, a porous self-supporting cathode for Li-CO 2 battery is fabricated through straightforward anchoring of two-dimensional (2D) cobalt-doped CeO 2 nanosheets on graphene aerogel , bypassing the addition of binder and the complicated manufacturing process. The combination of CeO 2 and Co 3 O 4 results in the reorganization of electronic structure by strongly coupled nanointerfaces, enhancing the reversible formation and decomposition of Li 2 CO 3 . Meanwhile, the unique porous structure facilitates the diffusion of CO 2 and electrolyte in Li-CO 2 batteries. The as-assembled Li-CO 2 battery achieves a superior discharge capacity (7860 mAh/g) and competitive cycling stability (>100 cycles). In particular, a flexible Li-CO 2 battery is developed with the freestanding cathode, which can provide a stable power output during multi-angle bending and folding. The improved conductivity, CO 2 adsorption ability and the electrochemical reaction pathway are revealed by density functional theory (DFT) calculations in detail. This work sheds new light on the development of advanced and flexible Li-CO 2 batteries for wearable electronics.