Nowadays, the efficient, stable,
and scalable conversion of solar
energy into chemical fuels represents a great scientific, economic,
and ethical challenge. Amongst the available candidate technologies,
photoelectrochemical water-splitting potentially has the most promising
technoeconomic trade-off between cost and efficiency. 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. 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.
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 [+0.602 V vs reversible
hydrogen electrode (RHE)] 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. 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.