Spatial Expansion of Catalytic Domains via Light-Driven Solid–Liquid Synergy for Advanced Li–S Batteries

Lithium–sulfur (Li–S) batteries hold great promise due to their high theoretical energy density yet are plagued by sluggish redox kinetics and the polysulfide shuttle effect. Here, we present a light-activated solid–liquid dual-phase catalytic system that addresses these challenges by integrating soluble cobalt phthalocyanine (CoPc) molecules into the electrolyte and anchoring CoPc/carbon nanotube (CNT) composites onto the cathode. This dual-phase architecture expands the catalytic region from the electrode surface into the bulk electrolyte, establishing a dynamic and spatially extended catalytic microenvironment. Upon light irradiation, photogenerated carriers trigger a cooperative catalytic process, where liquid-phase CoPc selectively adsorbs polysulfides, while solid-phase CoPc/CNT accelerates lithium sulfide (Li2S) nucleation and growth. This synergistic mechanism significantly enhances the electrochemical performance, enabling ultrastable cycling over 2000 cycles at 8C with a capacity decay of only 0.019% per cycle. Furthermore, excellent performance is maintained under practical conditions with high sulfur loading of 10.53 mg cm–2 and low electrolyte/sulfur ratio of 4 μL mg–1. This study demonstrates a scalable strategy for constructing spatiotemporally regulated catalytic domains, providing insights into the design of advanced photoassisted energy storage systems.