Photo‐Induced Dynamic Catalytic Domains for High‐Performance Lithium‐Sulfur Batteries

Abstract Lithium‐sulfur batteries (LSBs) face significant challenges due to sluggish reaction kinetics and the polysulfide shuttle effect. Here, a light‐induced anchoring strategy is employed to construct Co/Cu diatomic catalysts (DACs) on C₃N₄, introducing dual active sites with strong polysulfide adsorption and bifunctional catalytic activity. Upon light excitation, the synergistic Co–Cu interaction induces local electronic redistribution, which triggers broader electronic rearrangement and directional charge carrier migration. This process generates dynamic catalytic domains with enhanced polysulfide adsorption and catalytic conversion capability. These domains not only promote effective photogenerated carrier separation but also play a pivotal role in accelerating sulfur redox kinetics and regulating Li₂S deposition behavior. As a result, the Co/Cu‐C₃N₄ cathode exhibits exceptional electrochemical performance, achieving 1200 stable cycles at 8 C with a capacity decay of 0.025% per cycle. Remarkably, under lean electrolyte conditions (E/S = 4 µL mg⁻¹) and ultra‐high sulfur loading (14.73 mg cm⁻²), the battery maintains excellent cycling stability. This work offers a conceptual framework for photo‐induced catalytic microenvironment design and highlights the potential of spatiotemporal electronic modulation for next‐generation photo‐assisted energy storage systems.