Regulating Sulfur Redox Kinetics by Coupling Photocatalysis for High‐Performance Photo‐Assisted Lithium‐Sulfur Batteries

Abstract Challenges such as shuttle effect have hindered the commercialization of lithium‐sulfur batteries (LSBs), despite their potential as high‐energy‐density storage devices. To address these issues, we explore the integration of solar energy into LSBs, creating a photo‐assisted lithium‐sulfur battery (PA‐LSB). The PA‐LSB provides a novel and sustainable solution by coupling the photocatalytic effect to accelerate sulfur redox reactions. Herein, a perovskite quantum dot‐loaded MOF material serves as a cathode for the PA‐LSB, creating built‐in electric fields at the micro‐interface to extend the lifetime of photo‐generated charge carriers. The band structure of the composite material aligns well with the electrochemical reaction potential of lithium‐sulfur, enabling precise regulation of polysulfides in the cathode of the PA‐LSB system. This is attributed to the selective catalysis of the liquid‐solid reaction stage in the lithium‐sulfur electrochemical process by photocatalysis. These contribute to the outstanding performance of PA‐LSBs, particularly demonstrating a remarkably high reversible capacity of 679 mAh g −1 at 5 C, maintaining stable cycling for 1500 cycles with the capacity decay rate of 0.022 % per cycle. Additionally, the photo‐charging capability of the PA‐LSB holds the potential to compensate for non‐electric energy losses during the energy storage process, contributing to the development of lossless energy storage devices.