Robust nickel, manganese, and iron imidazole carboxylic acid catalysts for efficient visible-light driven reduction of CO2 to CO

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Three kinds of simple catalysts [Ni(H2L2)2(H2O)2] (Ni-IDC), [Mn(H2L2)2(H2O)2] (Mn-IDC) and [Fe(H2L2)2(H2O)2] (Fe-IDC) (H3L2 = 2-methyl-1-H-imidazole-4, 5-dicarboxylic acid) were synthesized with either nickel, manganese, or iron as the metal center, respectively. After 12 h of illumination, a turnover number (TON) for CO of 2264.8, with 95% selectivity, was achieved for Ni-IDC. High resolution mass spectrometry and the density functional theory calculations revealed that dimers of the complexes may play a role during the photocatalytic process. A mechanism involving two-stage proton-coupled electron transfer was proposed.