Exchange Coupling Determines Metal-Dependent Efficiency for Iron- and Cobalt-Catalyzed Photochemical CO2 Reduction
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A bs tract
Summary
A photochemical reduction of CO2 and CO to methane was shown using the nickel carbene complexes [Ni(bpy-bNHCMe)][PF6]2 (100831), [Ni(bpy)-(MeNHC)2][PF6]2 (100829), and [Ni(bpy-bNHCEt)][PF6]2 (100830) as catalysts in combination with the iridium-based photosensitizer Ir(ppy)3 (100843). Turnover numbers (TONs) up to 310000 for CO and 19000 for CH4 and selectivities of 90% for CO2 reduction products were reached for complex [Ni(bpy-bNHCEt)][PF6]2 (100830) in acetonitrile. The experiments were conducted under visible-light irradiation using BIH as sacrificial electron donor (see section SEDs below).
Advances and special progress
Additional remarks
The macrocyclic nickel carbene complex [Ni(bpy)-(MeNHC)2][PF6]2 (100829) gave a higher carbon-selective reduction percentage than the related complexes [Ni(bpy-bNHCEt)][PF6]2 (100830) and [Ni(bpy-bNHCMe)][PF6]2 (100831). The conversion of CO2 to CO and methane as well as the conversion of a CO/H2 atmosphere to methane were investigated with complex [Ni(bpy)-(MeNHC)2][PF6]2 (100829).
Content of the published article in detail
The article contains results for the reduction of CO2 to CO and CH4 and CO to CH4 under visible-light catalysis using a nickel complex as a catalyst. The catalytic system performs best (referring to the TON of CH4 production) in acetonitrile with a 1:1 CO/H2 atmosphere.
Catalysts tested in this study
Photosensitizer
Investigation
Further Information
The Supporting Information gives quantum yields for described experiments in Table 1.
Sacrificial electron donor
In this study, the experiments were done with the sacrificial electron donor BIH (100508).
Additives
Investigations
- CO2+ results from SI (Molecular process, Photocatalytic CO2 conversion experiments)
- CO2 Reduction under diverse conditions with diverse sensitizers (Molecular process, Photocatalytic CO2 conversion experiments)
- Iron-Catalyzed Photochemical CO2 Reduction under diverse conditions (Molecular process, Photocatalytic CO2 conversion experiments)
- Iron-Catalyzed Photochemical CO2 Reduction under diverse conditions error (Molecular process, Photocatalytic CO2 conversion experiments)
- Results Co2+ experiments taken from SI (Molecular process, Photocatalytic CO2 conversion experiments)
- Results obtained in a reaction with CO2+ catalyst (Assay, Cyclic Voltammetry experiments, Pages using duplicate arguments in template calls)
- Results obtained with Co2+ catalyst (Molecular process, Photocatalytic CO2 conversion experiments)
- Table 2 Co catalyst testing (Molecular process, Photocatalytic CO2 conversion experiments)
- Table 2 Conversion with Co catalyst (Molecular process, Photocatalytic CO2 conversion experiments)
- Table 2 conversion with Co catalyst (Molecular process, Photocatalytic CO2 conversion experiments)
- results CO2+ experiments (Molecular process, Photocatalytic CO2 conversion experiments)
- testtest2 (Molecular process, Photocatalytic CO2 conversion experiments)
