Boosting Active Species Ru‐O‐Zr/Ce Construction at the Interface of Phase‐Transformed Zirconia‐Ceria Isomerism toward Advanced Catalytic Cathodes for Li‐CO2 Batteries

Abstract Optimized structural support widely affects the improvement of interface structure, promoting the quantity and quality of active species simultaneously for Lithium battery cathodes. Herein, a highly dispersed and anchored active species at the interface of the Zr/CeO 2 (111) are achieved and are used for advanced Li‐CO 2 batteries cathodes. Benefiting from the abundant Ru‐O‐Zr/Ce site, the CO 2 adsorption and reduction is enhanced by the migration of the electron density in the C═O of CO 2 to Ru. The established Li‐CO 2 batteries exhibit excellent activity of 21 075 mAh g −1 and outstanding durability of over 167 cycles as well as low overpotential with 1.03 V at a discharge/recharge rate of 100 mA g −1 . The executed experiments combined with DFT calculations unveil that the cubic bimetallic oxide supported Ru exhibits optimized electronic structure at the interface compared to the monoclinic or tetragonal monometallic oxide support, promoting the increase of discharge voltage (from ≈2.5 to 2.73 V). Fundamentally, the redistribution of electron density on the active species Ru‐O‐Zr/Ce are intrinsic to above positive change, which are promoted by the synergistic interaction of Zr and Ce. This investigation provides an approach for the advancement of Li‐CO 2 batteries catalytic cathodes and for the promotion of “carbon neutral” goals.