Inorganic Chemistry, Journal Year: 2025, Volume and Issue: unknown
Published: April 14, 2025
Rechargeable lithium-carbon dioxide (Li-CO2) batteries are promising for CO2 capture and energy storage. However, the high decomposition potential sluggish kinetics of discharge product Li2CO3 limit their practical development. Recent studies have identified Li2C2O4 as an alternative with superior electrochemical properties. While nucleation mechanism has been well-studied, its remains unclear. This work comprehensively examines physical chemical differences between Li2C2O4. Both compounds exhibit insulating electronic structures, rapid lithium diffusion occurring in presence vacancies. Bonding analysis reveals that C-C covalent bonds within C2O4 groups key to differentiating two compounds. The weakly bonded group lowers Li2C2O4, allowing release without barrier after delithiation. Climbing image nudged elastic band calculations show results from cooperative dissociation CO3 groups. Ab initio molecular dynamics simulations indicate dissociates slowly delithiation, while simultaneously leading fast continuous study offers mechanistic insights into Li-CO2 products guides strategies enhance battery performance.
Language: Английский