Photocatalytic Reduction of CO2 by Highly Efficient Homogeneous FeII Catalyst based on 2,6-Bis(1’,2’,3’-triazolyl-methyl)pyridine. Comparison with Analogues.: Difference between revisions
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===Abstract=== | ===Abstract=== | ||
====Summary==== | ====Summary==== | ||
A photochemical reduction of CO<sub>2</sub> to CO was shown using the iron complex {{#moleculelink:|link=ZCGUPOIZKSBSCM-UHFFFAOYSA-N|image=false|width=300|height=200}} as catalyst in combination with the copper photosensitizer {{#moleculelink:|link= | A photochemical reduction of CO<sub>2</sub> to CO was shown using the iron complex {{#moleculelink:|link=ZCGUPOIZKSBSCM-UHFFFAOYSA-N|image=false|width=300|height=200}} as catalyst in combination with the copper photosensitizer {{#moleculelink: |link=QVCHJOOPCKCUBW-UHFFFAOYSA-P|image=false|width=300|height=200}}. 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 {{#moleculelink:|link=SIMPDUKIPFZEDX-UHFFFAOYSA-N|image=false|width=300|height=200}} and the cobalt complexes {{#moleculelink:|link=JDMNOCVBLMVSON-UHFFFAOYSA-N|image=false|width=300|height=200}} and {{#moleculelink:|link=QMZVNZOKJUBNLZ-UHFFFAOYSA-N|image=false|width=300|height=200}} were tested for CO<sub>2</sub> reduction as well, but did not show substantial conversion of CO<sub>2</sub> to CO. | ||
====Advances and special progress==== | ====Advances and special progress==== | ||
The authors reported a iron complex with one of the highest activities for CO<sub>2</sub> reduction among earth-abundant systems with monometallic iron catalysts. | The authors reported a iron complex with one of the highest activities for CO<sub>2</sub> reduction among earth-abundant systems with monometallic iron catalysts. | ||
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====Photosensitizer==== | ====Photosensitizer==== | ||
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-INDIGO- | -INDIGO-01102515052D | ||
0 0 0 0 0 0 0 0 0 0 0 V3000 | 0 0 0 0 0 0 0 0 0 0 0 V3000 | ||
M V30 BEGIN CTAB | M V30 BEGIN CTAB | ||
M V30 COUNTS | M V30 COUNTS 61 70 0 0 0 | ||
M V30 BEGIN ATOM | M V30 BEGIN ATOM | ||
M V30 1 C 12.15 -4.31795 0.0 0 | M V30 1 C 12.15 -4.31795 0.0 0 | ||
| Line 544: | Line 544: | ||
M V30 15 C 11.65 -6.91603 0.0 0 | M V30 15 C 11.65 -6.91603 0.0 0 | ||
M V30 16 C 12.15 -6.05 0.0 0 | M V30 16 C 12.15 -6.05 0.0 0 | ||
M V30 17 Cu 9.575 -4.05 0.0 0 | M V30 17 Cu 9.575 -4.05 0.0 0 CHG=1 | ||
M V30 18 C 7.81136 1.15012 0.0 0 | M V30 18 C 7.81136 1.15012 0.0 0 | ||
M V30 19 C 8.67693 -0.348124 0.0 0 | M V30 19 C 8.67693 -0.348124 0.0 0 | ||
| Line 584: | Line 584: | ||
M V30 55 C 12.9808 -4.7288 0.0 0 | M V30 55 C 12.9808 -4.7288 0.0 0 | ||
M V30 56 C 13.6926 -5.43137 0.0 0 | M V30 56 C 13.6926 -5.43137 0.0 0 | ||
M V30 57 B 15.5 0.25 0.0 0 CHG=-1 | |||
M V30 58 F 15.5 1.25 0.0 0 | |||
M V30 59 F 14.659 0.125 0.0 0 | |||
M V30 60 F 16.366 -0.25 0.0 0 | |||
M V30 61 F 15.5 -0.75 0.0 0 | |||
M V30 END ATOM | M V30 END ATOM | ||
M V30 BEGIN BOND | M V30 BEGIN BOND | ||
| Line 652: | Line 657: | ||
M V30 65 8 17 31 | M V30 65 8 17 31 | ||
M V30 66 8 17 32 | M V30 66 8 17 32 | ||
M V30 67 1 57 58 | |||
M V30 68 1 57 59 | |||
M V30 69 1 57 60 | |||
M V30 70 1 57 61 | |||
M V30 END BOND | M V30 END BOND | ||
M V30 END CTAB | M V30 END CTAB | ||
Revision as of 16:06, 10 January 2025
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 Molecule with key SIMPDUKIPFZEDX-UHFFFAOYSA-N does not exist. and the cobalt complexes 100944 and Molecule with key QMZVNZOKJUBNLZ-UHFFFAOYSA-N does not exist. 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. | 10 | 1.0 | 0.02 | 420 | 107 | 43 | ||||||||||||
| 2. | 10 | 1.0 | 0.02 | 420 | 109 | 54 | ||||||||||||
| 3. | 33 | 0.33 | 0.00666 | 420 | 238 | 137 | ||||||||||||
| 4. | 33 | 1.0 | 0.02 | 420 | 314 | 151 | ||||||||||||
| 5. | 10 | 1.0 | 0.02 | 420 | 576 | 287 | ||||||||||||
| 6. | 10 | 1.0 | 0.1 | 420 | 80 | 33 | ||||||||||||
| 7. | 10 | 1.0 | 0.02 | water | 420 | 7.4 | 6.4 | |||||||||||
| 8. | 10 | 1.0 | 0.02 | 420 | 3.2 | 1.6 | ||||||||||||
| 9. | 10 | 1.0 | 0.02 | 420 | 80 | 34 | ||||||||||||
| 10. | 10 | 1.0 | 0.02 | 420 | 100 | 43 | ||||||||||||
| 11. | 1.0 | 0.02 | 420 | 0 | 1 | |||||||||||||
| 12. | 10 | 0.02 | 420 | 0 | 0 | |||||||||||||
| 13. | 10 | 1.0 | 0.02 | 0 | 0 | |||||||||||||
| 14. | 10 | 1.0 | 0.02 | 420 | 0 | 0 | ||||||||||||
| 15. | 10 | 1.0 | 0.02 | Hg | 420 | 93 | 50 | |||||||||||
| 16. | 10 | 1.0 | 0.02 | solar simulator | 450 | 348 | ||||||||||||
| 17. | 10 | 1.0 | 420 | 6.8 | 0 | 0 | ||||||||||||
| 18. | 10 | 1.0 | 0.02 | 420 | 44 | 1.16 | 0 | |||||||||||
| 19. | 10 | 1.0 | 420 | 0 | 0 | 0 | ||||||||||||
| 20. | 10 | 1.0 | 0.02 | 420 | 0 | 0 | 0 |
Investigation-Name: Optimization of CO2 reduction conditions
| cat | cat conc [µM] | PS | PS conc [mM] | e-D | e-D conc [M] | solvent A | . | . | . | λexc [nm] | . | TON CO | TON H2 | . | |
|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|
| 1. | 100 | 1.0 | 0.02 | 420 | 7.8 | 2 | |||||||||
| 2. | 100 | 1.0 | 0.02 | 420 | 1.1 | 7.4 | |||||||||
| 3. | 100 | 1.0 | 0.02 | 420 | 0.7 | 4.9 |
Investigation-Name: CO2 reduction experiments testing different catalysts
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)
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