Reversible Li–CO2 batteries with a rare earth metal single-atom modified Janus structure: insights from an f-band center derived descriptor

Abstract

To address the sluggish kinetics of CO₂ 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.