Metal-Free Electron Donor-Acceptor Pair Enabled Long-Term Stability of Li-CO 2 Battery.

The challenges of Lithium-carbon dioxide (Li-CO 2 ) batteries for ensuring long-term cycling stability arise from the thermodynamically stable and electrically insulating discharge products (e.g., Li 2 CO 3 ), which primarily rely on their interaction with the active materials. To achieve the optimized intermediates, the bifunctional electron donor-acceptor (D-A) pairs are proposed in cathode design to adjust such interactions in the case of B-O pairs. The inclusion of BC 2 O sites allows for the optimized redistribution of electrons via p-π conjugation. The as-obtained D O -A B pairs endow the enhanced interactions with Li + , CO 2 , and various intermediates, accompanied by the adjustable growth mode of Li 2 CO 3 . The shift from solvation-mediated mode into surface absorption mode in turn manipulates the morphology and decomposition kinetics of Li 2 CO 3 . Therefore, the corresponding Li-CO 2 battery got twofold improved in both the capacity and reversibility. The cycling prolongs exceed 1300 h and well operates at a wide temperature range (20-50 °C) and different folding angles (0-180°). Such a strategy of introducing electron donor-acceptor pairs provides a distinct direction to optimize the lifetime of Li-CO 2 battery from local structure regulation at the atomic scale, further inspiring in-depth understandings for developing electrochemical energy storage and carbon capture technologies.