Xinyu Liu, Lu Liang, Jin Ren, Huilin Liu, Jiale Wan, Xiaolin Guo, Yueyao Dong, Hang Qi, Yizhe Meng, Shuwei Hao, Chunhui Yang, Yunfei Shang, Liwei Dong
Integrated photo-assisted rechargeable batteries have emerged as a highly promising strategy for solar-to-chemical energy conversion. However, the rapid recombination of photocarriers under intense ion flux fails to provide an additional driving force to promote both interfacial charge transfer and lithium-ion (Li+) diffusion, thereby severely constraining their high-rate capability due to sluggish overall kinetics. Herein, we propose a universal photo-assisted strategy utilizing non-planar titanium oxo phthalocyanine (TiOPc) as a stable photosensitizer. The out-of-plane asymmetry and electron-withdrawing Ti[double bond, length as m-dash]O bond of TiOPc induce a pronounced molecular dipole. This unique molecular configuration effectively mitigates intermolecular aggregation and drives efficient exciton dissociation, thereby suppressing carrier recombination and steering photocarriers to the interface to accelerate both charge-transfer and Li+ diffusion kinetics. Consequently, the TiOPc-sensitized LiFePO4 cathode delivers a 72.1% capacity enhancement under illumination at 8C compared to dark conditions. Furthermore, this photo-assisted strategy is well compatible with layered oxide cathodes and sodium battery systems. This work establishes a rational molecular-engineering paradigm to overcome the inherent kinetic limitations of next-generation fast-charging light-responsive energy storage by suppressing photocarrier recombination.