Stabilized 2‐Electron Oxalate Mechanism Enabled by Oriented 3D Mo 1.33 C MXene/rGO Catalyst for Enhanced Reversibility in Flexible Li‐CO 2 Batteries

Abstract The incomplete decomposition of Li 2 CO 3 significantly impacts the reversible performance of lithium‐carbon dioxide (Li‐CO 2 ) batteries. Current catalysts reported so far can promote the decomposition of Li 2 CO 3 to a certain extent, but are far from sufficient, and the modulation of the discharge product to the more decomposable Li 2 C 2 O 4 is a promising solution. However, Li 2 C 2 O 4 exhibits insufficient stability for prolonged cycling processes. Herein, a Mo 1.33 C@rGO aerogel (MGA), an all‐integrated flexible cathode catalyst, is prepared for Li‐CO 2 batteries, where an abundance of mobile electrons produced by the organized Mo vacancies strengthens the bonding between Mo atoms and the intermediate C 2 O 4 2 − , thereby stabilizing it during prolonged cycling and preventing its disproportionation into Li 2 CO 3 . 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 Li 2 C 2 O 4 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 Li 2 C 2 O 4 decomposition, offering a promising pathway for efficient, long‐lasting, advanced Li‐CO 2 batteries.