Light‐Driven Polymer‐Based All‐Solid‐State Lithium‐Sulfur Battery Operating at Room Temperature

Abstract Poly(ethylene oxide)‐based polymer all‐solid‐state LiS battery is a promising candidate due to its high specific energy, good processability, and low cost. However, the poor room temperature ionic conductivity limits its further development. Here an innovative photothermal battery technology is proposed to realize the normal operation at room temperature. This design places the 3D Cu substrate with Cu/Si core‐shell structures between Li anode and outer encapsulation glass, so that the light can come in and generate heat efficiently by utilizing the carrier nonradiative recombination of Si nano shell, then the heat quickly transfers to the battery system through Cu core. Once simulated sunlight irradiates, the battery achieves a fast reaction kinetics and superior photothermal conversion, thus realizing a lifespan of over 20 cycles with a capacity of 1089.9 mAh g⁻¹ at 0.2 C. Even on the actual sunlight irradiation, a high discharge/charge capacity of 1065.2/1036.5 mAh g⁻¹ is also reached, indicating an excellent reversible electrochemical process. Moreover, the 3D nanostructure can accommodate the fatal volume variation of lithium and reduce the effective current density, thus suppressing the dendrite nucleation and growth. This study will open the avenue to develop a room temperature polymer all‐solid‐state LiS battery using photothermal technology.