Catalyzed carbon-based materials for CO₂-battery utilization

Increasing atmospheric CO₂ levels and global carbon neutrality goals have driven interest in technologies that both mitigate CO₂ emissions and provide sustainable energy storage solutions. Metal-carbon dioxide (M-CO₂) batteries offer significant promise due to their high energy density and potential to utilize atmospheric CO₂. A key challenge in advancing M-CO₂ batteries lies in optimizing CO₂-breathing cathodes, which are essential for CO₂ adsorption, diffusion, and conversion. Carbon-based cathodes play a critical role in facilitating CO₂ redox for M-CO₂ batteries, owing to their cost-effectiveness, high conductivity, tunable microstructure, and porosity. However, there is a lack of current systematic understanding of the relationship between the structure, composition, and catalytic properties of carbon-based cathodes, as well as their impact on the overall efficiency, stability, and durability of M-CO₂ batteries. In this review, we will give an insightful review and analysis of recent advances in various carbon-based materials, including commercial carbons, single-atom catalysts, transition metal/carbon composites, metal-organic frameworks, etc., focusing on their structure-function-property relationships. A comprehensive understanding of the pivotal role played by carbon-based materials and their optimization strategies in M-CO₂ batteries will be provided. Moreover, future perspectives and research suggestions for carbon-based materials are presented to advance the development and innovation of M-CO₂ batteries.