2023
DOI: 10.1021/jacs.3c11206
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Infrared Spectroscopic Observation of Oxo- and Superoxo-Intermediates in the Water Oxidation Cycle of a Molecular Ir Catalyst

Hongna Zhang,
Boqiang Chen,
Tianying Liu
et al.

Abstract: Molecular Ir catalysts have emerged as an important class of model catalysts for understanding structure−activity relationships in water oxidation, a reaction that is central to renewable fuel synthesis. Prior efforts have mostly focused on controlling and elucidating the emergence of active species from prepared precursors. However, the development of efficient and stable molecular Ir catalysts also necessitates probing of reaction intermediates. To date, relatively little is known about the key intermediates… Show more

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Cited by 7 publications
(7 citation statements)
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“…They are ascribed to the O–O and O–C–O stretching modes within [Fe–O–O–R], respectively (see the SI for detailed discussions). ,,, The reversibility of these signals with changing potentials was further confirmed by filtering out static background absorbance with phase sensitive detection (Figure S27). The successful detection of the [Fe–O–O–R] intermediate lends additional strong support to the proposed mechanisms. It is important to note that the nucleophilic attack by the M-OOH species on the substrate is the key enabling factor for the Baeyer–Villiger oxidation.…”
Section: Resultsmentioning
confidence: 89%
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“…They are ascribed to the O–O and O–C–O stretching modes within [Fe–O–O–R], respectively (see the SI for detailed discussions). ,,, The reversibility of these signals with changing potentials was further confirmed by filtering out static background absorbance with phase sensitive detection (Figure S27). The successful detection of the [Fe–O–O–R] intermediate lends additional strong support to the proposed mechanisms. It is important to note that the nucleophilic attack by the M-OOH species on the substrate is the key enabling factor for the Baeyer–Villiger oxidation.…”
Section: Resultsmentioning
confidence: 89%
“…A pseudo-first-order characteristic was thus observed relative to the cyclohexanone concentration. By comparison, at low applied potentials, a relatively slow H 2 O oxidation is expected, implying a relatively low coverage of surface *OOH species . In this case, the overall reaction rate would be largely determined by the availability of surface *>OOH species (Figure c) .…”
Section: Resultsmentioning
confidence: 96%
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