![]() ![]() (11-14) By taking advantage of scientific know-how, large material availability, and technological solutions that have already been developed in the organic PV field, efficient organic photocathodes have been demonstrated, (15, 16) reaching, in some cases, performances comparable with their inorganic counterparts. ![]() (5-10) It is only very recently that polymer-based devices for photoelectrochemical hydrogen production have been reported by a few groups. (4) In contrast with the PV field, exploitation of the optoelectronic properties of conjugated polymers for photoelectrochemical applications has been scarcely considered. (3) One of the main advantages of polymer semiconductors is their compatibility with flexible devices, as well as with solution-processed, large area deposition techniques. (1, 2) Recently, a power conversion efficiency of over 10% has been achieved by the most efficient conjugated polymer semiconductors in state-of-the-art organic PV cells. Organic semiconductors have attracted considerable interest in cost-effective electricity generation using third-generation photovoltaics (PVs). The demonstrated all solution-processed hybrid photoelectrodes represent an eligible candidate for the scalable and low-cost solar-to-H 2 conversion technology that embodies the feasibility requirements for large area, plant-scale applications. The sequential deposition of inorganic material, charge-selective contacts, visible-light sensitive organic polymers, and earth-abundant, nonprecious catalyst by spin coating leads to state-of-the-art photoelectrochemical parameters, comprising a high onset potential and a positive maximum power point (+0.222 V vs RHE), a photocurrent density as high as 5.25 mA/cm 2 at 0 V versus RHE, an incident photon-to-current conversion efficiency at 0 V versus RHE of above 35%, and 100% faradaic efficiency for hydrogen production. ![]() Here, we report for the first time an all solution-processed approach for the fabrication of hybrid organic/inorganic photocathodes based on organic semiconductor bulk heterojunctions that exhibit promising photoelectrochemical performance. However, research on semiconductors and photoelectrode architectures suitable for H 2 evolution has focused mainly on the use of fabrication techniques and inorganic materials that are not easily scalable. Amongst the available candidate technologies, photoelectrochemical water-splitting potentially has the most promising technoeconomic trade-off between cost and efficiency. Nowadays, the efficient, stable, and scalable conversion of solar energy into chemical fuels represents a great scientific, economic, and ethical challenge. ![]()
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