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=SVWABAAUBHILMW-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). | 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=SVWABAAUBHILMW-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. | ||
====Additional remarks==== | ====Additional remarks==== | ||
In addition to the production of CO, a substantial amount of H<sub>2</sub> was formed in the reduction process with | In addition to the production of CO, a substantial amount of H<sub>2</sub> (TON of 287) was formed in the reduction process with complex {{#moleculelink:|link=ZCGUPOIZKSBSCM-UHFFFAOYSA-N|image=false|width=300|height=200}}. | ||
===Content of the published article in detail=== | ===Content of the published article in detail=== | ||
The article contains results for the reduction of CO<sub>2</sub> to CO under visible-light catalysis using | The article contains results for the reduction of CO<sub>2</sub> to CO under visible-light catalysis using the iron complex {{#moleculelink:|link=ZCGUPOIZKSBSCM-UHFFFAOYSA-N|image=false|width=300|height=200}} as a catalyst. The catalytic system performs best (referring to the TON of CO production) in MeCN/TEOA. | ||
====Catalyst==== | ====Catalyst==== | ||
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-INDIGO-05142414222D | |||
0 0 0 0 0 0 0 0 0 0 0 V3000 | |||
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M V30 END ATOM | |||
M V30 BEGIN BOND | |||
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M V30 2 2 5 3 | |||
M V30 3 1 2 6 | |||
M V30 4 1 3 4 | |||
M V30 5 2 6 7 | |||
M V30 6 1 7 5 | |||
M V30 7 1 2 8 | |||
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M V30 20 1 19 11 | |||
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M V30 25 1 20 25 | |||
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M V30 28 1 26 24 | |||
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M V30 34 1 31 29 | |||
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M V30 37 1 32 36 | |||
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M V30 49 1 45 40 | |||
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M V30 58 1 50 54 | |||
M V30 59 2 56 51 | |||
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M V30 68 1 61 53 | |||
M V30 69 8 34 1 | |||
M V30 70 8 46 1 | |||
M V30 71 8 1 45 | |||
M V30 72 8 15 1 | |||
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M V30 END BOND | M V30 END BOND | ||
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====Investigation==== | ====Investigation==== | ||
{{#experimentlist: |form=Photocatalytic_CO2_conversion_experiments|name=Optimization of CO2 reduction conditions|importFile=}} | |||
{{#experimentlist:|form=Photocatalytic_CO2_conversion_experiments|name=CO2 reduction experiments testing different catalysts|importFile=}} | |||
====Sacrificial electron donor==== | ====Sacrificial electron donor==== | ||
In this study, the experiments were done with the sacrificial electron donor BIH ([[Molecule:100508|100508]]). | In this study, the experiments were done with the sacrificial electron donor BIH ([[Molecule:100508|100508]]). | ||
====Additives==== | ====Additives==== | ||
In this study, control experiments with Hg and without CO<sub>2</sub> were conducted. | In this study, control experiments with Hg and without CO<sub>2</sub> were conducted. |
Latest revision as of 14:03, 16 May 2024
Abstract[edit | edit source]
Summary[edit | edit source]
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[edit | edit source]
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[edit | edit source]
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[edit | edit source]
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[edit | edit source]
Photosensitizer[edit | edit source]
Investigation[edit | edit source]
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 |
cat | cat conc [µM] | PS | PS conc [mM] | e-D | e-D conc [M] | solvent A | . | . | . | λexc [nm] | . | TON CO | TON H2 | . | |
---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|
1. | 0.1 | 1.0 | 0.02 | 420 | 7.8 | 2 | |||||||||
2. | 0.1 | 1.0 | 0.02 | 420 | 1.1 | 7.4 | |||||||||
3. | 0.1 | 1.0 | 0.02 | 420 | 0.7 | 4.9 |
Sacrificial electron donor[edit | edit source]
In this study, the experiments were done with the sacrificial electron donor BIH (100508).
Additives[edit | edit source]
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)