Journal
ENERGY & ENVIRONMENTAL SCIENCE
Volume 2, Issue 2, Pages 230-238Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/b818708h
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Funding
- U. S. Department of Energy [DE-FG02-07ER15909]
- NERSC
- NSF [CHE-0215926, 0404191]
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Inexpensive water oxidation catalysts are needed to develop photocatalytic solar cells that mimic photosynthesis and produce fuel from sunlight and water. This paper reports the successful attachment of a dinuclear di-mu-oxo manganese water oxidation catalyst [H2O(terpy)Mn-III(mu-O)(2) Mn-IV(terpy)H2O](NO3)(3) (1, terpy = 2,2':6'2 ''-terpyridine) onto TiO2 nanoparticles (NPs) via direct adsorption, or in situ synthesis. The resulting surface complexes are characterized by EPR and UV-visible spectroscopy, electrochemical measurements and computational modeling. We conclude that the mixed-valence (III, IV) state of 1 attaches to near-amorphous TiO2 NPs by substituting one of its water ligands by the TiO2 NP, as suggested by low-temperature (7 K) EPR data. In contrast, the analogous attachment onto well-crystallized TiO2 NPs leads to dimerization of 1 forming Mn(IV) tetramers on the TiO2 surface as suggested by EPR spectroscopy and electrochemical studies.
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