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

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

Author information

1
Department of Chemistry, Merkert Chemistry Center, Boston College, 2609 Beacon St., Chestnut Hill, MA 02467 (USA).
2
Department of Chemistry, Yale University, 225 Prospect Street, PO Box 208107, New Haven, CT 06520-8107 (USA).
3
Department of Chemistry and Biochemistry, Worcester Polytechnic Institute, 100 Institute Road, Worcester, MA 01609 (USA).
4
Department of Chemistry, Yale University, 225 Prospect Street, PO Box 208107, New Haven, CT 06520-8107 (USA). gary.brudvig@yale.edu.
5
Department of Chemistry, Merkert Chemistry Center, Boston College, 2609 Beacon St., Chestnut Hill, MA 02467 (USA). dunwei.wang@bc.edu.

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

PMID:
26184365
DOI:
10.1002/anie.201504427

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