Redox potentials of high-valent iron-, cobalt-, and nickel-oxido complexes: evidence for exchange enhanced reactivity
The ferrocene titration method has been employed to determine the one-electron reduction potentials of a series of oxido-iron(IV), oxido-cobalt(IV) and oxido/hydroxido-nickel(III) complexes based on the same tetradentate TMG3tren ligand (TMG3tren=tris[2-(N-tetramethylguanidyl)ethyl]amine). The S=2 g...
Gespeichert in:
| Hauptverfasser: | , , , |
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| Dokumenttyp: | Article (Journal) |
| Sprache: | Englisch |
| Veröffentlicht: |
2020
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| In: |
Israel journal of chemistry
Year: 2020, Jahrgang: 60, Heft: 10/11, Pages: 957-962 |
| ISSN: | 1869-5868 |
| DOI: | 10.1002/ijch.202000038 |
| Online-Zugang: | Verlag, kostenfrei, Volltext: https://doi.org/10.1002/ijch.202000038 Verlag, kostenfrei, Volltext: https://onlinelibrary.wiley.com/doi/abs/10.1002/ijch.202000038 
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| Verfasserangaben: | Peter Comba, Anna-Maria Löhr, Florian Pfaff, and Kallol Ray |
MARC
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| 245 | 1 | 0 | |a Redox potentials of high-valent iron-, cobalt-, and nickel-oxido complexes |b evidence for exchange enhanced reactivity |c Peter Comba, Anna-Maria Löhr, Florian Pfaff, and Kallol Ray |
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| 520 | |a The ferrocene titration method has been employed to determine the one-electron reduction potentials of a series of oxido-iron(IV), oxido-cobalt(IV) and oxido/hydroxido-nickel(III) complexes based on the same tetradentate TMG3tren ligand (TMG3tren=tris[2-(N-tetramethylguanidyl)ethyl]amine). The S=2 ground state of the [(TMG3tren)FeIV=O]2+ complex allows an exchange enhanced reactivity, which enables it to perform efficient oxygen atom transfer (OAT) and hydrogen atom abstraction (HAA) reactions with a low one-electron reduction potential of 270 mV vs. SCE. In the absence of exchange enhanced reactivity, the OAT and HAA abilities of the S=3/2 [(TMG3tren)CoIV−O(Sc(OTf)3)]2+, S=1/2 [(TMG3tren)NiIII−O(H)]2+ and the previously reported S=1 [(TMC)(CH3CN)FeIV=O]2+ and [(N4Py)FeIV=O]2+ complexes can be directly correlated to their reduction potentials. Notably, [(N4Py)FeIV=O]2+ and [(TMG3tren)FeIV=O]2+ exhibit similar OAT and HAA reactivities although the reduction potential of [(N4Py)FeIV=O]2+ is 0.24 V more positive than that of [(TMG3tren)FeIV=O]2+. The present study therefore provides experimental evidence for exchange enhanced reactivity and rationalizes nature's choice for employing S=2 oxido-iron(IV) cores to achieve difficult oxidation reactions at biologically viable potentials. | ||
| 650 | 4 | |a exchange enhanced reactivity | |
| 650 | 4 | |a high-valent metal-oxido complexes | |
| 650 | 4 | |a late transition metals | |
| 650 | 4 | |a non heme iron | |
| 650 | 4 | |a reduction potential | |
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| 700 | 1 | |a Pfaff, Florian Felix |d 1985- |e VerfasserIn |0 (DE-588)1079564756 |0 (DE-627)841236429 |0 (DE-576)452800641 |4 aut | |
| 700 | 1 | |a Ray, Kallol |d 1978- |e VerfasserIn |0 (DE-588)130265896 |0 (DE-627)496582445 |0 (DE-576)29809620X |4 aut | |
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