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Chemical and Spectroscopic Evidence for an Fe V -Oxo Complex
Abstract
Iron(V)-oxo species have been proposed as key reactive intermediates in the catalysis of oxygen-activating enzymes and synthetic catalysts. Here, we report the synthesis of [Fe(TAML)(O)] – in nearly quantitative yield, where TAML is a macrocyclic tetraamide ligand. Mass spectrometry, Mössbauer, electron paramagnetic resonance, and x-ray absorption spectroscopies, as well as reactivity studies and density functional theory calculations show that this long-lived (hours at –60°C) intermediate is a spin S = 1/2 iron(V)-oxo complex. Iron-TAML systems have proven to be efficient catalysts in the decomposition of numerous pollutants by hydrogen peroxide, and the species we characterized is a likely reactive intermediate in these reactions.
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Cites
Structure and chemistry of cytochrome p450
Denisov, I. G., Makris, T. M., Sligar, S. G., & Schlichting, I. (2005) · Chemical Reviews · doi:10.1021/cr0307143 · Cited by 2,106
Cited by
Ghosh, A. (2017) · Chemical Reviews · doi:10.1021/acs.chemrev.6b00590 · Cited by 359
Why did Nature choose manganese to make oxygen?
Armstrong, F. A. (2008) · Philosophical Transactions of the Royal Society B: Biological Sciences · doi:10.1098/rstb.2007.2223 · Cited by 204
Nandy, A., Zhu, J., Janet, J. P., Duan, C., Getman, R. B., & Kulik, H. J. (2019) · ACS Catalysis · doi:10.1021/acscatal.9b02165 · Cited by 91
Metadata
- Authors
- de Oliveira, F. T., Chanda, A., Banerjee, D., Shan, X., Mondal, S., Que, L., Bominaar, E. L., Münck, E., & Collins, T. J.
- Venue
- Science
- Published
- 2007-02-09
- Volume
- 315
- Issue
- 5813
- Pages
- 835-838
- ISSN
- 0036-8075 (ISSN-L)
- 1095-9203
- OpenAlex
- W1970522028
- Cited by
- 490
- References
- 1
- FWCI
- 14.42
- Type
- journal article
- Language
- en
- Open access
- closed
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- de Oliveira, F. T., Chanda, A., Banerjee, D., Shan, X., Mondal, S., Que, L., Bominaar, E. L., Münck, E., & Collins, T. J. (2007). Chemical and Spectroscopic Evidence for an Fe V -Oxo Complex. Science. https://doi.org/10.1126/science.1133417
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