Issue 6, 2023

Evaluation of CH4 oxidation activity of high-valent iron-oxo species of a μ-nitrido-bridged heterodimer of iron porphycene and iron phthalocyanine

Abstract

A μ-nitrido-bridged dimer of iron phthalocyanine is one of the most potent molecule-based CH4 oxidation catalysts reported to date. The reactive intermediate is a high-valent iron-oxo species generated through reaction with H2O2 in an acidic aqueous solution. However, there are few reports on the synthesis and catalytic CH4 oxidation activity of a μ-nitrido-bridged heterodimer of two different iron porphyrinoids, despite that there are a variety of iron porphyrinoids with coordination and electronic structures different from those of iron phthalocyanines or iron porphyrins. Herein, we report the synthesis of a novel μ-nitrido-bridged heterodimer of an iron phthalocyanine and iron porphycene and examine its CH4 oxidation activity. Porphycenes are an important class of porphyrinoids with a smaller coordination sphere than phthalocyanines or porphyrins. Single crystal structural analyses revealed that the heterodimer possessed a Fe–N[double bond, length as m-dash]Fe core structure similar to that of the phthalocyanine homodimer. The heterodimer showed catalytic CH4 oxidation activity in an acidic aqueous solution in the presence of H2O2 at 60 °C through the high-valent iron-oxo species as in the case with the phthalocyanine homodimer. This was in clear contrast to the result that the high-valent iron-oxo species of a μ-nitrido-bridged iron porphycene dimer was so unstable that it decomposed quickly in the same reaction conditions.

Graphical abstract: Evaluation of CH4 oxidation activity of high-valent iron-oxo species of a μ-nitrido-bridged heterodimer of iron porphycene and iron phthalocyanine

Supplementary files

Article information

Article type
Paper
Submitted
19 Nov. 2022
Accepted
30 Janv. 2023
First published
31 Janv. 2023

Catal. Sci. Technol., 2023,13, 1725-1734

Author version available

Evaluation of CH4 oxidation activity of high-valent iron-oxo species of a μ-nitrido-bridged heterodimer of iron porphycene and iron phthalocyanine

Y. Yamada, Y. Miwa, Y. Toyoda, Q. M. Phung, K. Oyama and K. Tanaka, Catal. Sci. Technol., 2023, 13, 1725 DOI: 10.1039/D2CY01980A

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