Photocatalytic Reduction of CO2 by Highly Efficient Homogeneous FeII Catalyst based on 2,6-Bis(1’,2’,3’-triazolyl-methyl)pyridine. Comparison with Analogues.
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Abstract
Summary
A photochemical reduction of CO2 to CO was shown using the iron complex 100941 as catalyst in combination with the copper photosensitizer 100940. Turnover numbers (TONs) of 576 and a selectivity of 67% for CO were reached in MeCN/TEOA. The experiments were conducted under visible-light irradiation (λ = 420 nm) using BIH as sacrificial electron donor (see section SEDs below). The homoleptic iron complex 100942 and the cobalt complexes 100944 and 100945 were tested for CO2 reduction as well, but did not show substantial conversion of CO2 to CO.
Advances and special progress
The authors reported a iron complex with one of the highest activities for CO2 reduction among earth-abundant systems with monometallic iron catalysts.
Additional remarks
In addition to the production of CO, a substantial amount of H2 (TON of 287) was formed in the reduction process with complex 100941.
Content of the published article in detail
The article contains results for the reduction of CO2 to CO under visible-light catalysis using the iron complex 100941 as a catalyst. The catalytic system performs best (referring to the TON of CO production) in MeCN/TEOA.
Catalyst
Photosensitizer
Investigation
| cat | cat conc [µM] | PS | PS conc [mM] | e-D | e-D conc [M] | solvent A | . | . | additives | . | . | λexc [nm] | . | TON CO | TON CH4 | TON H2 | . | |
|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|
| 1. | 0.1 | 1.0 | 0.02 | 420 | 107 | 43 | ||||||||||||
| 2. | 0.1 | 1.0 | 0.02 | 420 | 109 | 54 | ||||||||||||
| 3. | 0.03 | 0.33 | 0.00666 | 420 | 238 | 137 | ||||||||||||
| 4. | 0.03 | 1.0 | 0.02 | 420 | 314 | 151 | ||||||||||||
| 5. | 0.01 | 1.0 | 0.02 | 420 | 576 | 287 | ||||||||||||
| 6. | 0.1 | 1.0 | 0.1 | 420 | 80 | 33 | ||||||||||||
| 7. | 0.1 | 1.0 | 0.1 | water | 420 | 7.4 | 6.4 | |||||||||||
| 8. | 0.1 | 1.0 | 0.02 | 420 | 3.2 | 1.6 | ||||||||||||
| 9. | 0.1 | 1.0 | 0.02 | 420 | 80 | 34 | ||||||||||||
| 10. | 0.1 | 1.0 | 0.02 | 420 | 100 | 43 | ||||||||||||
| 11. | 1.0 | 0.02 | 420 | 0 | 1 | |||||||||||||
| 12. | 0.1 | 0.02 | 420 | 0 | 0 | |||||||||||||
| 13. | 0.1 | 1.0 | 0.02 | 0 | 0 | |||||||||||||
| 14. | 0.1 | 1.0 | 0.02 | 420 | 0 | 0 | ||||||||||||
| 15. | 0.1 | 1.0 | 0.02 | Hg | 420 | 93 | 50 | |||||||||||
| 16. | 0.1 | 1.0 | 0.02 | solar simulator | 450 | 348 | ||||||||||||
| 17. | 0.01 | 1.0 | 420 | 6.8 | 0 | 0 | ||||||||||||
| 18. | 0.01 | 1.0 | 0.02 | 420 | 44 | 1.16 | 0 | |||||||||||
| 19. | 0.01 | 1.0 | 420 | 0 | 0 | 0 | ||||||||||||
| 20. | 0.01 | 1.0 | 0.02 | 420 | 0 | 0 | 0 |
Sacrificial electron donor
In this study, the experiments were done with the sacrificial electron donor BIH (100508).
Additives
In this study, control experiments with Hg and without CO2 were conducted.
Investigations
- CO2 reduction experiments testing different catalysts (Molecular process, Photocatalytic CO2 conversion experiments)
- Optimization of CO2 reduction conditions (Molecular process, Photocatalytic CO2 conversion experiments)
