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 11 2022
Accepted
30 1 2023
First published
31 1 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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