Abstract
The lithium-carbon dioxide (Li-CO(2)) battery is a promising energy storage technology that integrates CO(2) utilization with energy storage and conversion. However, its development is hindered by slow reaction kinetics and insulating Li(2)CO(3) discharge products deposited at the cathode, which cause severe polarization and rapid capacity degradation. Herein, novel Cu-based catalysts with multiple active sites anchored on nitrogen-doped carbon (Cu/NC) are developed to achieve highly efficient Li-CO(2) batteries. Metallic Cu nanoparticles facilitate efficient electron transfer during the CO(2) reduction reaction (CO(2)RR), while the induced Cu-N/O dual active sites effectively reduce the energy barrier for decomposing discharge products. Furthermore, the optimized N configurations in the NC matrix enhance the intrinsic activity of the catalytic sites. Consequently, the Li-CO(2) battery incorporating the optimized catalyst demonstrates attractive cycling stability over 850 h at 300 mA g(-1), with a remarkably low overpotential of 1.30 V, showing great potential for low-cost and highly efficient Li-CO(2) batteries. This work provides a strategic route for designing cost-effective multi-active-site catalysts, offering critical insights into the development of high-performance Li-CO(2) batteries.