Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 138, Issue 47, Pages 15291-15294Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.6b08532
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Funding
- MINECO
- FEDER [CTQ2016-80058-R, SEV-2013-0319, CTQ2014-52974-REDC]
- EU COST Actions [CM1202, CM1205]
- U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES), CSGB Division [DE-AC02-06CH11357]
- U.S. DOE
- Canadian Light Source
- U.S. NSF [CHE-1361595]
- U.S. DOE, Basic Energy Sciences, under SciDAC [DE-SC0008666]
- Russian Ministry of Education and Science [14.587.21.0002, RFMEFI58714X0002]
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An end-on superoxido complex with the formula {[Co-III(OH2) (trpy)] [Co-III(OO center dot) (trpy) (mu-bpp)}(4+) (3(4+)) (bpp(-) = bis(2-pyridyl)-3,5-pyrazolate; trpy = 2,2';6':2 ''-terpyridine) has been characterized by resonance Raman, electron paramagnetic resonance, and X-ray absorption spectroscopies. These results together with online mass spectrometry experiments using O-17 and O-18 isotopically labeled compounds prove that this compound is a key intermediate of the water oxidation reaction catalyzed by the peroxido-bridged complex {[Co-III(trpy)](2)(mu-bpp) (mu-OO)}(3+) (1(3+)). DFT calculations agree with and complement the experimental data, offering a complete description of the transition states and intermediates involved in the catalytic cycle.
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