Complementary Weaknesses: A Win‐Win Approach for rGO/CdS to Improve the Energy Conversion Performance of Integrated Photorechargeable Li‐S Batteries

Integrating solar energy into rechargeable battery systems represents a significant advancement towards sustainable energy storage solutions. Herein, we propose a win‐win solution to reduce the shuttle effect of polysulfide and improve the photocorrosion stability of CdS, thereby enhancing the energy conversion efficiency of rGO/CdS‐based photorechargeable integrated lithium‐sulfur batteries (PRLSBs). Experimental results show that CdS can effectively anchor polysulfide under sunlight irradiation for 20 minutes. Under a high current density (1 C), the discharge‐specific capacity of the PRLSBs increased to 971.30 mA h g‐1, which is 113.3% enhancement compared to that of under dark condition (857.49 mA h g‐1). Remarkably, without an electrical power supply, the PRLSBs can maintain a 21 hours discharge process following merely 1.5 hours of light irradiation, achieving a breakthrough solar‐to‐electrical energy conversion efficiency of up to 5.04%. Ex‐situ X‐ray photoelectron spectroscopy (XPS) and in‐situ Raman analysis corroborate the effectiveness of this complementary weakness approach in bolstering redox kinetics and curtailing polysulfide dissolution in PRLSBs. This work showcases a feasible strategy to develop PRLSBs with potential dual‐functional metal sulfide photoelectrodes, which will be of great interest in future‐oriented off‐grid photocell systems.