Song, ZeyuWu, JihuaiTu, YongguangSun, LiuxueZhu, TingtingLi, GuodongWang, XiaobingDu, YitianDeng, ChunyanChen, QiSun, WeihaiHuang, MiaoliangFan, LeqingHuang, YunfangWei, YuelinXie, YimingLin, YuChen, HongweiLin, JianmingZhan, LanGao, PengNazeeruddin, Mohammad KhajaHuang, Wei2022-09-122022-09-122022-09-122022-09-0110.1039/d2ee01744jhttps://infoscience.epfl.ch/handle/20.500.14299/190732WOS:000849196300001Photocapacitor integrating both energy harvest and storage functions into a single device is a frontier research orientation, which facilitates the efficient and sustainable utilization of green energy. However, the multi-functions in one device and structural complexity of the integrated device, particularly the mismatch between energy harvest and storage units, lead to a relatively large energy loss in the energy storage and output processes. Here, we design a voltage adjustable hybrid supercapacitor (VAHSC) as an energy storage unit of a three-terminal photocapacitor. The VAHSC effectively harmonizes the energy harvest and storage units, resulting in the current, voltage, power, and energy match between both units. The optimal photocapacitor achieves a storage efficiency as high as 98.28% and Joule efficiency of 86.01%, along with excellent charge/discharge cycle stability. The great leap in this efficiency marks a substantial step towards the practical application of solar-charging energy storage integrated devices.Chemistry, MultidisciplinaryEnergy & FuelsEngineering, ChemicalEnvironmental SciencesChemistryEnergy & FuelsEngineeringEnvironmental Sciences & Ecologystoragecapacitorsystemdeviceconversiondesigntext::journal::journal article::research article