Stimuli Responsive Rechargeable Li-CO₂ Batteries

Lithium-carbon dioxide (Li-CO₂) batteries represent a promising approach for integrating electrochemical energy storage with CO₂ utilization. However, their practical implementation is fundamentally constrained by sluggish reaction kinetics and the high thermodynamic stability of discharge products, resulting in large overpotential, catalyst deactivation, interfacial instability, and limited reversibility. Conventional catalyst and electrolyte engineering have only partially addressed these challenges, prompting the exploration of dynamic strategies that actively regulate the reaction environment. External stimuli, including light irradiation, pressure, and piezoelectric polarization, provides such an approach by modulating electronic structure, interfacial energetics, charge-transfer pathways, and local reaction environments. These effects accelerate reaction kinetics, promote reversible formation and decomposition, suppress electrode passivation, and improve the overall electrochemical performance. In this review, we first discuss the fundamental reaction mechanisms of Li-CO₂ batteries and the thermodynamic and kinetic origins of their performance limitations. We then systematically examine the working mechanisms of diverse stimuli-assisted strategies, critically comparing their electrochemical roles, advantages, limitations, energy requirements, and practical applicability from a unified mechanistic perspective. Finally, we identify the key scientific and engineering challenges that remain and outline future directions for the rational design of efficient, durable, and scalable stimuli-assisted Li-CO₂ batteries.