Rear‐Illuminated Perovskite Photorechargeable Lithium Battery

Abstract Photovoltaic power‐conversion systems can harvest energy from sunlight almost perpetually whenever sunrays are accessible. Meanwhile, as indispensable energy storage units used in advanced technologies such as portable electronics, electric vehicles, and renewable/smart grids, batteries are energy‐limited closed systems and require constant recharging. Fusing these two essential technologies into a single device would create a sustainable power source. Here, it is demonstrated that such an integrated device can be realized by fusing a rear‐illuminated single‐junction perovskite solar cell with Li 4 Ti 5 O 12 ‐LiCoO 2 Li‐ion batteries, whose photocharging is enabled by an electronic converter via voltage matching. This design facilitates a straightforward monolithic stacking of the battery on the solar cell using a common metal substrate, which provides a robust mechanical isolation between the two systems while simultaneously providing an efficient electrical interconnection. This system delivers a high overall photoelectric conversion‐storage efficiency of 7.3%, outperforming previous efforts on stackable integrated architectures with organic–inorganic photovoltaics. Furthermore, converter electronics facilitates system control with battery management and maximum power point tracking, which are inevitable for efficient, safe, and reliable operation of practical loads. This work presents a significant advancement toward integrated photorechargeable energy storage systems as next‐generation power sources.