Rhenium(I) trinuclear rings as highly efficient redox photosensitizers for photocatalytic CO2 reduction: Difference between revisions
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===Abstract=== | ===Abstract=== | ||
==== Summary==== | ==== Summary==== | ||
A photochemical reduction of CO<sub>2</sub> to CO or formic acid was shown using the bipyridine-based catalysts {{#moleculelink:|link=NZCMNMSVXYOMGS-UHFFFAOYSA-N|image=false|width=300|height=200}}, {{#moleculelink:|link=XUQJAKJUMNDNTK-UHFFFAOYSA-L|image=false|width=300|height=200}} or {{#moleculelink:|link= | A photochemical reduction of CO<sub>2</sub> to CO or formic acid was shown using the bipyridine-based rhenium, ruthenium and manganese catalysts {{#moleculelink:|link=NZCMNMSVXYOMGS-UHFFFAOYSA-N|image=false|width=300|height=200}}, {{#moleculelink:|link=XUQJAKJUMNDNTK-UHFFFAOYSA-L|image=false|width=300|height=200}} or {{#moleculelink:|link=WCQGNVNGTWFVLO-UHFFFAOYSA-N|image=false|width=300|height=200}} in combination with cyclic rhenium-based trinuclear redox photosensitizers . Turnover numbers (TONs) of up to 290 for formic acid and up to 98 for CO were reached in DMF or DMA. The experiments were conducted under visible-light irradiation (λ = 436 nm) using TEOA as sacrificial electron donor (see section SEDs below). | ||
====Advances and special progress==== | ====Advances and special progress==== | ||
====Additional remarks==== | ====Additional remarks==== | ||
===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 or formic acid under visible-light catalysis using | The article contains results for the reduction of CO<sub>2</sub> to CO or formic acid under visible-light catalysis using bipyridine-based complexes and rhenium-based trinuclear rings as photosensitizers. The catalytic system performs best (referring to the TON of formate production) in DMA and in DMF for CO production. | ||
==== Catalyst==== | ==== Catalyst==== | ||
<chemform smiles="C1C=C2C3C=CC=CN=3[Re+]([C-]#[O+])([C-]#[O+])([C-]#[O+])(N#CC)N2=CC=1.[P-](F)(F)(F)(F)(F)F" inchi="1S/C10H8N2.C2H3N.3CO.F6P.Re/c1-3-7-11-9(5-1)10-6-2-4-8-12-10;1-2-3;3*1-2;1-7(2,3,4,5)6;/h1-8H;1H3;;;;;/q;;;;;-1;+1" inchikey="NZCMNMSVXYOMGS-UHFFFAOYSA-N" height="200px" width="300px" float="none"> | <chemform smiles="C1C=C2C3C=CC=CN=3[Re+]([C-]#[O+])([C-]#[O+])([C-]#[O+])(N#CC)N2=CC=1.[P-](F)(F)(F)(F)(F)F" inchi="1S/C10H8N2.C2H3N.3CO.F6P.Re/c1-3-7-11-9(5-1)10-6-2-4-8-12-10;1-2-3;3*1-2;1-7(2,3,4,5)6;/h1-8H;1H3;;;;;/q;;;;;-1;+1" inchikey="NZCMNMSVXYOMGS-UHFFFAOYSA-N" height="200px" width="300px" float="none"> | ||
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Abstract
Summary
A photochemical reduction of CO2 to CO or formic acid was shown using the bipyridine-based rhenium, ruthenium and manganese catalysts [Re(bpy)(CO)3(MeCN)][PF6], Ru(dtBubpy)(CO)2Cl2 or Molecule with key WCQGNVNGTWFVLO-UHFFFAOYSA-N does not exist. in combination with cyclic rhenium-based trinuclear redox photosensitizers . Turnover numbers (TONs) of up to 290 for formic acid and up to 98 for CO were reached in DMF or DMA. The experiments were conducted under visible-light irradiation (λ = 436 nm) using TEOA as sacrificial electron donor (see section SEDs below).
Advances and special progress
Additional remarks
Content of the published article in detail
The article contains results for the reduction of CO2 to CO or formic acid under visible-light catalysis using bipyridine-based complexes and rhenium-based trinuclear rings as photosensitizers. The catalytic system performs best (referring to the TON of formate production) in DMA and in DMF for CO production.
Catalyst
[Re(bpy)(CO)3(MeCN)][PF6]
Ru(dtBubpy)(CO)2Cl2
Photosensitizer
Investigation
| cat | cat conc [µM] | PS | PS conc [mM] | solvent A | . | . | λexc [nm] | . | TON CO | . | . | . | |
|---|---|---|---|---|---|---|---|---|---|---|---|---|---|
| 1. | 0.05 | 0.05 | 436 | 27 | |||||||||
| 2. | 0.05 | 0.05 | 436 | 98 | |||||||||
| 3. | 0.05 | 0.05 | 436 | 22 | |||||||||
| 4. | 0.05 | 0.05 | 436 | 71 | |||||||||
| 5. | 0.05 | 436 | 6 | ||||||||||
| 6. | 0.05 | 436 | 8 | ||||||||||
| 7. | 0.05 | 0.05 | 436 | 20 | |||||||||
| 8. | 0.05 | 0.05 | 436 | 32 | |||||||||
| 9. | 0.05 | 0.05 | 436 | 11 | |||||||||
| 10. | 0.05 | 0.05 | 436 | 48 |
Investigation-Name: Table 1
| cat | cat conc [µM] | PS | PS conc [mM] | e-D | e-D conc [M] | solvent A | . | . | λexc [nm] | . | TON CO | TON H2 | TON HCOOH | . | . | . | |
|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|
| 1. | 0.05 | 0.05 | 436 | 20 | 72 | 290 | |||||||||||
| 2. | 0.05 | 0.05 | 0.03 | 436 | 16 | 49 | 280 | ||||||||||
| 3. | 0.05 | 0.05 | 436 | 32 | 85 | ||||||||||||
| 4. | 0.05 | 0.05 | 0.03 | 436 | 80 | 60 |
Investigation-Name: Table 2
Sacrificial Electron Donor
In this study, the experiments were done with the sacrificial electron donor TEOA (100507).
Additives
In this study, no additives were tested.
