Journal
JOURNAL OF CATALYSIS
Volume 307, Issue -, Pages 140-147Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2013.07.018
Keywords
Ruthenium catalyst; Water oxidation; Surface-binding; Photoisomerization
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Funding
- Brookhaven National Laboratory (BNL) [DE-AC02-98CH10886]
- U.S. Department of Energy
- Division of Chemical Sciences, Geosciences, & Biosciences, Office of Basic Energy Sciences
- U.S. Department of Energy, Office of Basic Energy Sciences
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Surface-binding of molecular water oxidation catalysts through phosphonated ligands offers a promising strategy for attaching homogeneous catalysts onto conductive or semiconductive oxide surfaces for heterogeneous catalysis. In this work, the highly active [Ru(tpy)(pynap)OH2](2+) (tpy = 2,2':6',2 ''-terpyridine; pynap = 2-(pyrid-2'-yl)-1,8-naphthyridine) water oxidation catalyst is attached onto metal oxide electrodes through a phosphate group. Electrochemical and photoelectrochemical results confirm that ruthenium oxidation chemistries and water oxidation proficiency remain largely unaffected by phosphonation. Surface-binding reveals minimal photoisomerization of the active d-form and allows us to evaluate photoelectrochemical and mechanistic properties of the catalyst. Spectroelectrochemical experiments support the evolution of multiple ruthenium oxidation states in agreement with Pourbaix diagrams. Although photoisomerization of d-[Ru(H2PO3-tpy)(pynap)OH2](2+) is considerably hindered when the catalyst is attached onto a rigid oxide electrode, surface desorption remains a major challenge. (C) 2013 Elsevier Inc. All rights reserved.
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