Perovskite Solar Cells Based on Polymerized Chlorophyll Films as Environmentally Friendly Hole-Transporting Layers

Hole-transporting layers (HTLs) play a crucial role in the performance of inverted, p-i-n perovskite solar cells (PSCs). Chlorophylls (Chls) are naturally abundant organic photoconductors on earth, with good charge carrier mobility and appropriate Fermi energy levels that make them promising candidates for use in photovoltaic devices. However, Chls films prepared using the solution method exhibit lower carrier mobility compared to other organic polymer films, which limits their application in PSCs. To address this issue, Chls molecules are chemically linked to reduce the charge transfer barrier, thus the transfer of charges between molecules is transformed to intramolecular charge transfer. This study synthesizes and characterizes two polymerized Chl films, PolyCuChl and PolyNiChl, as HTLs of CH3NH3PbI3-based PSCs. PSCs based on the electrochemical polymerization of PolyChl HTLs demonstrate an enhanced power conversion efficiency (PCE) of up to 19.0%, which is the highest efficiency among devices based on Chl materials. Furthermore, these devices demonstrated exceptional long-term stability. These results highlight the potential of polymerized Chl films as a viable alternative to conventional HTLs in PSCs. The approach utilizes abundant, environmentally friendly, and versatile Chl derivatives, and can be extended to develop next-generation HTL materials for improved PSC performance. Hole-transporting layers are essential for inverted perovskite solar cells (PSCs). Natural chlorophylls (Chl) show potential, while their solution-based films suffer from low carrier mobility. To address this, PolyChl films are synthesized via electrochemical polymerization and applied to CH3NH3PbI3 PSCs, achieving a record-high efficiency of 19.0% among Chl-based devices.image