Photocatalytic CO2 reduction with aminoanthraquinone organic dyes
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Abstract
Summary
The photochemical reduction of CO2 to CO was shown using the iron complex Fe(DHPP)Cl in combination with the aminoanthraquinone photosensitizers 1-aminoanthraquinone, 1-amino-4-hydroxyanthraquinone, 1-Amino-2-bromo-4-hydroxyanthraquinone, Bromaminic acid, 1,2-Diaminoanthraquinone and 1,4-Diaminoanthraquinone. Turnover numbers (TONs) of up to 21616 and a selectivity of >99.9% for CO were reached in DMF after 48 h of irradiation. The experiments were conducted under visible-light irradiation (λ > 400 nm) with BIH (see section SEDs below) as sacrificial electron donor.
Advances and special progress
The authors present an efficient photocatalytic system with naturally abundant photosensitizers and without rare metals in which both the photosensitizer and catalyst show a high activity.
Additional remarks
For the most efficient system investigated in this study, a TON of 21616 per mole of catalyst and a TON of 6012 per mole of photosensitizer was obtained.
Content of the published article in detail
The article contains results of a study for the reduction of CO2 to CO using an iron complex and different aminoanthraquinone-based photosensitizers. The catalytic system performs best (referring to the TON of CO production) in DMF with photosensitizer 1-Amino-2-bromo-4-hydroxyanthraquinone.
Catalyst
Photosensitizer
Investigation
| cat | cat conc [µM] | PS | PS conc [mM] | e-D | e-D conc [M] | solvent A | λexc [nm] | . | TON CO | . | . | |
|---|---|---|---|---|---|---|---|---|---|---|---|---|
| 1. | 0.0006 | 0.02 | 0.06 | >400 | 2395 | |||||||
| 2. | 0.0006 | 0.02 | 0.06 | >400 | 2738 | |||||||
| 3. | 0.0006 | 0.02 | 0.06 | >400 | 3551 | |||||||
| 4. | 0.0006 | 0.02 | 0.06 | >400 | 8360 | |||||||
| 5. | 0.0006 | 0.02 | 0.06 | >400 | 21616 | |||||||
| 6. | 0.0006 | 0.02 | 0.06 | >400 | 907 |
| cat | cat conc [µM] | PS | PS conc [mM] | e-D | e-D conc [M] | solvent A | λexc [nm] | TON CO | . | |
|---|---|---|---|---|---|---|---|---|---|---|
| 1. | 0.0005 | 0.0005 | 0.06 | > 400 | 3174 | |||||
| 2. | 0.001 | 0.001 | 0.06 | > 400 | 3587 | |||||
| 3. | 0.002 | 0.002 | 0.06 | > 400 | 3817 | |||||
| 4. | 0.005 | 0.005 | 0.06 | > 400 | 4978 | |||||
| 5. | 0.01 | 0.01 | 0.06 | > 400 | 4028 | |||||
| 6. | 0.0005 | 0.02 | 0.06 | > 400 | 19158 | |||||
| 7. | 0.0006 | 0.02 | 0.06 | > 400 | 21616 | |||||
| 8. | 0.001 | 0.02 | 0.06 | > 400 | 17020 | |||||
| 9. | 0.002 | 0.02 | 0.06 | > 400 | 11250 | |||||
| 10. | 0.01 | 0.02 | 0.06 | > 400 | 3942 | |||||
| 11. | 0.02 | 0.02 | 0.06 | > 400 | 2134 | |||||
| 12. | 0.05 | 0.02 | 0.06 | > 400 | 891 | |||||
| 13. | 0.002 | 0.015 | 0.06 | > 400 | 8772 | |||||
| 14. | 0.002 | 0.01 | 0.06 | > 400 | 5593 | |||||
| 15. | 0.005 | 0.01 | 0.06 | > 400 | 4128 | |||||
| 16. | 0.01 | 0.01 | 0.06 | > 400 | 4028 | |||||
| 17. | 0.02 | 0.01 | 0.06 | > 400 | 2325 | |||||
| 18. | 0.002 | 0.005 | 0.06 | > 400 | 8780 | |||||
| 19. | 0.005 | 0.005 | 0.06 | > 400 | 5258 | |||||
| 20. | 0.01 | 0.005 | 0.06 | > 400 | 2576 | |||||
| 21. | 0.02 | 0.005 | 0.06 | > 400 | 1539 |
Sacrificial electron donor
In this study, the experiments were done with the sacrificial electron donor BIH (100508).
Additives
In this study, the addition of Hg(0) was tested.
Investigations
- Photocatalytic CO2 reduction with varying concentrations of cat and PS (Molecular process, Photocatalytic CO2 conversion experiments)
- Photocatalytic reduction of CO2 with different photosensitizers (Molecular process, Photocatalytic CO2 conversion experiments)
