Photoelectrochemical water splitting by hybrid organic-inorganic systems: setting the path from 2% to 20% solar-to-hydrogen conversion efficiency

Promoting solar fuels as a viable alternative to hydrocarbons calls for technologies that couple efficiency, durability, and low cost. In this work we elucidate how hybrid organic-inorganic systems employing hybrid photocathodes (HPC) and perovskite solar cells (PSC) could eventually match these needs, enabling sustainable and clean hydrogen production. First, we demonstrate a system comprising an HPC, a PSC, and a Ru-based oxygen evolution catalyst reaching a solar-to-hydrogen (STH) efficiency above 2%. Moving from this experimental result, we elaborate a perspective for this technology by adapting the existing models to the specific case of an HPC-PSC tandem. We found two very promising scenarios: one with a 10% STH efficiency, achievable using the currently available semiconducting polymers and the widely used methylammonium lead iodide (MAPI) PSC, and the other one with a 20% STH efficiency, requiring dedicated development for water-splitting applications of recently reported high-performing organic semiconductors and narrow band-gap perovskites.