Authors: Xue Tian, Huan Liu, Bin Cao, Peng Zhang, Ruihong Zhang, Razium A. Soomro, Haonan Cui, Bin Xu
Published: 2025-05-30
Source: Full article
AbstractThe incomplete decomposition of Li2CO3 significantly impacts the reversible performance of lithium‐carbon dioxide (Li‐CO2) batteries. Current catalysts reported so far can promote the decomposition of Li2CO3 to a certain extent, but are far from sufficient, and the modulation of the discharge product to the more decomposable Li2C2O4 is a promising solution. However, Li2C2O4 exhibits insufficient stability for prolonged cycling processes. Herein, a Mo1.33C@rGO aerogel (MGA), an all‐integrated flexible cathode catalyst, is prepared for Li‐CO2 batteries, where an abundance of mobile electrons produced by the organized Mo vacancies strengthens the bonding between Mo atoms and the intermediate C2O42−, thereby stabilizing it during prolonged cycling and preventing its disproportionation into Li2CO3. At the same time, the oriented 3D framework of MGA provides ordered active sites and well‐organized electron and ion transport channels, reducing charge transfer resistance and facilitating the decomposition of Li2C2O4 with a minimal overpotential of 0.46 V, extending the cycle lifespan to 330 cycles at a current density of 20 µA cm−2. These results highlight MGA's potential as a catalyst for stabilizing intermediates and promoting Li2C2O4 decomposition, offering a promising pathway for efficient, long‐lasting, advanced Li‐CO2 batteries.