Reversible Li-CO batteries with a rare earth metal single-atom modified Janus structure: insights from an f-band center derived descriptor.

To address the sluggish kinetics of CO reduction and release reactions and poor cycling stability in lithium-carbon dioxide batteries, this study proposes a bifunctional catalyst based on a rare-earth monometallic catalyst anchored with Janus MoSSe. Through density functional theory calculations and transition state analysis, the Dy-S@MoSSe catalyst was selected with a total overpotential of only 1.00 V, which is superior to graphene and commercial carbon nanotubes. The f-d electron coupling effect reduces the activation energy of the key step and optimizes the adsorption energy of the intermediate. The descriptors constructed based on the d-f orbital synergy show a strong linear correlation with the overpotential, providing a universal theoretical framework for the design of high-performance catalysts and promoting the application of rare-earth monometallic materials in carbon-based technologies.