▎ 摘　　要

Carbonyl compounds with elements of C, H, and O and reversible redox-active centers are promising electrode materials in rechargeable batteries owing to their high theoretical capacity, structure flexibility and resources abundance. However, the low conductivity and the dissolution of active molecules in organic electrolyte limit the practical application. Immobilizing the carbonyls on graphene provides a simple approach to address these two issues. However, most reported interaction between carbon-based substrates and carbonyl compounds is weak pi-pi interaction, which is not strong enough to prohibit the detachment of active materials from carbon surface, and thus leading to undesirable cycling performance. Herein, we applied the first principle calculations to study the carbonyls-graphene interaction and found that the weak pi-pi interaction can be rationally converted to the strong pi-Li-pi interaction via introducing the groups containing Li atoms. The introduced Li atoms can cooperatively bind with the two aromatic pi components through the covalent Li-carbonyl compounds interaction and Li-graphene interaction. The concept of pi-Li-pi interaction provides a versatile method to suppress the dissolution of active materials and increase the electronic conductivity at the same time, which gains insight into the design of organic electrode materials for rechargeable batteries with high performance.