Methane Formation Induced via Face-to-Face Orientation of Cyclic Fe Porphyrin Dimer in Photocatalytic CO2 Reduction

Author:

Kuramochi Yusuke12ORCID,Hashimoto Masaya1,Satake Akiharu12

Affiliation:

1. Department of Chemistry, Graduate School of Science, Tokyo University of Science, 1-3 Kagurazaka, Shinjuku-ku, Tokyo 162-8621, Japan

2. Department of Chemistry, Faculty of Science Division II, Tokyo University of Science, 1-3 Kagurazaka, Shinjuku-ku, Tokyo 162-8621, Japan

Abstract

Iron porphyrins are known to provide CH4 as an eight-electron reduction product of CO2 in a photochemical reaction. However, there are still some aspects of the reaction mechanism that remain unclear. In this study, we synthesized iron porphyrin dimers and carried out the photochemical CO2 reduction reactions in N,N-dimethylacetamide (DMA) containing a photosensitizer in the presence of 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole (BIH) as an electron donor. We found that, despite a low catalytic turnover number, CH4 was produced only when these porphyrins were facing each other. The close proximity of the cyclic dimers, distinguishing them from a linear Fe porphyrin dimer and monomers, induced multi-electron CO2 reduction, emphasizing the unique role of their structural arrangement in CH4 formation.

Funder

JSPS KAKENHI

ENEOS Hydrogen Trust Fund

Publisher

MDPI AG

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