Exchange Coupling Determines Metal-Dependent Efficiency for Iron- and Cobalt-Catalyzed Photochemical CO2 Reduction
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Abstract
Summary
A photochemical reduction of CO2 to CO was shown using an Fe2+ and Co2+ complexes as catalysts in combination with Ruxx as photosensitizer.
metal−ligand exchange coupling as an example of charge delocalization that can determine the efficiency for photocatalytic CO2RR. A comparative evaluation of iron and cobalt complexes supported by the redox-active ligand tpyPY2Me establishes that the two-electron reduction of [Co(tpyPY2Me)]2+ ([Co]2+) occurs at potentials 770 mV more negative than the [Fe(tpyPY2Me)]2+ ([Fe]2+) analogue by maximizing the exchange coupling in the latter compound.
Advances and special progress
Additional remarks
Content of the published article in detail
Catalysts tested in this study
Photosensitizer
Ru(bpy)3
3,6-Diamino-10-methylacridinium
100971
Ir(ppy)3
Investigation
| cat | cat conc [µM] | PS | PS conc [mM] | e-D | e-D conc [M] | . | . | solvent A | additives | . | . | TON CO | TON H2 | . | . | |
|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|
| 1. | 2 | 0.2 | 0.1 | 15520 | 86 | |||||||||||
| 2. | 0.2 | 0.2 | 0.1 | 30349 | 1013 | |||||||||||
| 3. | 0.2 | 0.1 | 43 | 52 | ||||||||||||
| 4. | 2 | 0.1 | 112 | 0 | ||||||||||||
| 5. | 2 | 0.2 | 150 | 0 | ||||||||||||
| 6. | 2 | 0.2 | 0.1 | 6 | 0 | |||||||||||
| 7. | 2 | 0.2 | 0.1 | Ar | 0 | 222 | ||||||||||
| 8. | 2 | 0.2 | 0.1 | 12749 | 163 | |||||||||||
| 9. | 0.2 | 0.2 | 0.1 | 28712 | 6527 | |||||||||||
| 10. | 2 | 0.2 | 0.1 | 18502 | 141 | |||||||||||
| 11. | 2 | 0.2 | 0.1 | 6710 | 0 |
| cat | cat conc [µM] | PS | PS conc [mM] | e-D | e-D conc [M] | . | . | solvent A | additives | . | . | TON CO | TON H2 | . | . | |
|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|
| 1. | 2 | 0.2 | 0.1 | 15520 | 86 | |||||||||||
| 2. | 0.2 | 0.2 | 0.1 | 30349 | 1013 | |||||||||||
| 3. | 0.2 | 0.1 | 43 | 52 | ||||||||||||
| 4. | 2 | 0.1 | 112 | 0 | ||||||||||||
| 5. | 2 | 0.2 | 150 | 0 | ||||||||||||
| 6. | 2 | 0.2 | 0.1 | 6 | 0 | |||||||||||
| 7. | 2 | 0.2 | 0.1 | Ar | 0 | 222 | ||||||||||
| 8. | 2 | 0.2 | 0.1 | 12749 | 163 | |||||||||||
| 9. | 0.2 | 0.2 | 0.1 | 28712 | 6527 | |||||||||||
| 10. | 2 | 0.2 | 0.1 | 18502 | 141 | |||||||||||
| 11. | 2 | 0.2 | 0.1 | 6710 | 0 |
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 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)
- 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)
