Abstract
Solar batteries capable of harvesting sunlight and storing solar energy present an attractive vista to transition our energy infrastructure into a sustainable future. Here we present an integrated, fully earth-abundant solar battery based on a bifunctional (light absorbing and charge storing) carbon nitride (K-PHI) photoanode, combined with organic hole transfer and storage materials. An internal ladder-type hole transfer cascade via a transport layer is used to selectively shuttle the photogenerated holes to the PEDOT:PSS cathode. This concept differs from previous designs such as light-assisted battery schemes or photocapacitors and allows charging with light during both electrical charge and discharge, thus substantially increasing the energy output of the cell. Compared to battery operation in the dark, light-assisted (dis)charging increases charge output by 243%, thereby increasing the electric coulombic efficiency from 68.3% in the dark to 231%, leading to energy improvements of 94.1% under illumination. This concept opens new vistas towards compact, highly integrated devices based on multifunctional, carbon-based electrodes and separators, and paves the way to a new generation of earth-abundant solar batteries.