Directional migration and efficient separation of charge carriers in photo-assisted batteries enabled by optical and magnetic regulation

Photo-assisted rechargeable batteries exhibit excellent electrochemical performance, attributed to their unique photoenhancement effect. However, their performance is constrained by low utilization efficiency of photogenerated carriers in the cathode material. We herein realize the targeted modulation of photogenerated electron selectivity with the aim of maximizing the lithium storage capacity per unit time by constructing a metal–organic coordination system. This system integrates magnetic cobalt (Co) centers, 2,2′-bipyridine photoactive units, and two specific storage ligands (i.e., DHBQ and BQ). Upon photoexcitation, the strong ligand-to-ligand charge transfer (LLCT) effect facilitates electron transfer between different lithium-storage ligands. Furthermore, the application of an external magnetic field extends the photogenerated carrier lifetime and improves separation efficiency by modulating spin-polarized carriers and enhancing spin–orbit coupling, which further enhances LLCT. Benefiting from the combined modulation of illumination and magnetic field, the organic cathode delivers a discharge capacity of 416 mAh g −1 . This work not only provides new insights into the dynamics of photogenerated carriers in battery cathodes but also offers valuable guidance for the development of multi-field regulated energy storage systems.