Catalytic H2O2 Activation by a Diiron Complex for Methanol Oxidation.

Zimmermann TP, Orth N, Finke S, Limpke T, Stammler A, Bögge H, Walleck S, Ivanovic-Burmazovic I, Glaser T (2020)
Inorganic chemistry 59(21): 15563–15569.

Zeitschriftenaufsatz | Veröffentlicht | Englisch
 
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Autor*in
Zimmermann, Thomas Philipp; Orth, Nicole; Finke, SebastianUniBi; Limpke, Thomas; Stammler, AnjaUniBi; Bögge, HartmutUniBi; Walleck, StephanUniBi; Ivanovic-Burmazovic, Ivana; Glaser, ThorstenUniBi
Abstract / Bemerkung
In nature, C-H bond oxidation of CH4 involves a peroxo intermediate that decays to the high-valent active species of either a "closed" {FeIV(mu-O)2FeIV} core or an "open" {FeIV(O)(mu-O)FeIV(O)} core. To mimic and to obtain more mechanistic insight in this reaction mode, we have investigated the reactivity of the bioinspired diiron complex [(susan){Fe(OH)(mu-O)Fe(OH)}]2+ [susan = 4,7-dimethyl-1,1,10,10-tetrakis(2-pyridylmethyl)-1,4,7,10-tetraazadecane], which catalyzes CH3OH oxidation with H2O2 to HCHO and HCO2H. The kinetics is faster in the presence of a proton. 18O-labeling experiments show that the active species, generated by a decay of the initially formed peroxo intermediate [(susan){FeIII(mu-O)(mu-O2)FeIII}]2+, contains one reactive oxygen atom from the mu-oxo and another from the mu-peroxo bridge of its peroxo precursor. Considering an FeIVFeIV active species, a "closed" {FeIV(mu-O)2FeIV} core explains the observed labeling results, while a scrambling of the terminal and bridging oxo ligands is required to account for an "open" {FeIV(O)(mu-O)FeIV(O)} core.
Erscheinungsjahr
2020
Zeitschriftentitel
Inorganic chemistry
Band
59
Ausgabe
21
Seite(n)
15563–15569
eISSN
1520-510X
Page URI
https://pub.uni-bielefeld.de/record/2948415

Zitieren

Zimmermann TP, Orth N, Finke S, et al. Catalytic H2O2 Activation by a Diiron Complex for Methanol Oxidation. Inorganic chemistry. 2020;59(21):15563–15569.
Zimmermann, T. P., Orth, N., Finke, S., Limpke, T., Stammler, A., Bögge, H., Walleck, S., et al. (2020). Catalytic H2O2 Activation by a Diiron Complex for Methanol Oxidation. Inorganic chemistry, 59(21), 15563–15569. https://doi.org/10.1021/acs.inorgchem.0c02698
Zimmermann, T. P., Orth, N., Finke, S., Limpke, T., Stammler, A., Bögge, H., Walleck, S., Ivanovic-Burmazovic, I., and Glaser, T. (2020). Catalytic H2O2 Activation by a Diiron Complex for Methanol Oxidation. Inorganic chemistry 59, 15563–15569.
Zimmermann, T.P., et al., 2020. Catalytic H2O2 Activation by a Diiron Complex for Methanol Oxidation. Inorganic chemistry, 59(21), p 15563–15569.
T.P. Zimmermann, et al., “Catalytic H2O2 Activation by a Diiron Complex for Methanol Oxidation.”, Inorganic chemistry, vol. 59, 2020, pp. 15563–15569.
Zimmermann, T.P., Orth, N., Finke, S., Limpke, T., Stammler, A., Bögge, H., Walleck, S., Ivanovic-Burmazovic, I., Glaser, T.: Catalytic H2O2 Activation by a Diiron Complex for Methanol Oxidation. Inorganic chemistry. 59, 15563–15569 (2020).
Zimmermann, Thomas Philipp, Orth, Nicole, Finke, Sebastian, Limpke, Thomas, Stammler, Anja, Bögge, Hartmut, Walleck, Stephan, Ivanovic-Burmazovic, Ivana, and Glaser, Thorsten. “Catalytic H2O2 Activation by a Diiron Complex for Methanol Oxidation.”. Inorganic chemistry 59.21 (2020): 15563–15569.

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