LAUSR

Abstract Rechargeable Li-CO2 batteries (LCBs) are considered as a promising candidate for the next generation energy storage system, but still be impeded by the lack of high-performance cathode catalyst and poor understanding for the complicated reaction mechanism. In the present work, we demonstrate that the catalytic capability of cathode catalyst of LCBs can be remarkably enhanced from the accelerated reaction kinetics using a p-type substrate as adsorption/desorption promoter for refined reaction route. A carbon-free atomic Ir-Te cathode catalyst with Ir atomic cluster is uniformly super-assembled on the surface of Te nanowires forming an amorphous surface layer (ca. 3 nm) to maximize the catalytic capability of active Ir sites and provide a refined reaction pathway due to synergistic effect of Ir active sites and Te substrate. The adsorption ability of Li2C2O4 during discharging and the desorption ability of CO2 species during charging of the p-type Te substrate could both promote the catalytic reaction kinetics and optimize the reaction pathways on Ir active sites. Finally, a large specific capacity of 13,247.1 mAh g−1 and an excellent high rate cyclability with stably over 350 and 200 cycles at the current density of 1000 and 2000 mA g−1 are achieved. This contribution provides a rational design strategy for high performance cathode catalyst, and intrinsic insight towards the understanding the reaction mechanisms of LCBs.