Hematite-Based Solar Water Splitting in Acidic Solutions: Functionalization by Mono- and Multilayers of Iridium Oxygen-Evolution Catalysts

Angew Chem Int Ed Engl. 2015 Sep 21;54(39):11428-32. doi: 10.1002/anie.201504427. Epub 2015 Jul 15.

Abstract

Solar water splitting in acidic solutions has important technological implications, but has not been demonstrated to date in a dual absorber photoelectrochemical cell. The lack of functionally stable water-oxidation catalysts (WOCs) in acids is a key reason for this slow development. The only WOCs that are stable at low pH are Ir-based systems, which are typically too expensive to be implemented broadly. It is now shown that this deficiency may be corrected by applying an ultra-thin monolayer of a molecular Ir WOC to hematite for solar water splitting in acidic solutions. The turn-on voltage is observed to shift cathodically by 250 mV upon the application of a monolayer of the molecular Ir WOC. When the molecular WOC is replaced by a heterogeneous multilayer derivative, stable solar water splitting for over 5 h is achieved with near-unity Faradaic efficiency.

Keywords: hematite; homogeneous catalysis; iridium; photoelectrochemistry; solar water splitting.