Metal-free reduction of CO2 to formate using a photochemical organohydride-catalyst recycling strategy: Difference between revisions
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===Abstract=== | ===Abstract=== | ||
====Summary==== | ====Summary==== | ||
A photochemical reduction of CO<sub>2</sub> to CO was shown using | A photochemical reduction of CO<sub>2</sub> to CO was shown using {{#moleculelink:|link=|image=|width=|height=}} as catalyst in combination with the organic carbazole-based photosensitizer {{#moleculelink:|link=SEAGXMGVRJVEBS-UHFFFAOYSA-N|image=false|width=300|height=200}}. Turnover numbers (TONs) of 6080 for the catalyst and 8820 for the photosensitizer and an exclusive selectivity for formic acid were reached in MeCN/H<sub>2</sub>O with catalyst xx. The experiments were conducted under visible-light irradiation (λ = 400 nm) using ascorbic acid 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 | The article contains results for the reduction of CO<sub>2</sub> to HCOO<sup>-</sup> under visible-light catalysis using as a catalyst. The catalytic system performs best (referring to the TON of formic acid production) in MeCN/H<sub>2</sub>O. | ||
====Catalyst==== | ====Catalyst==== | ||
<chemform smiles="C1C=CC2N(C)C(C)=[N+](C)C=2C=1.[I-]" inchi="1S/C10H13N2.HI/c1-8-11(2)9-6-4-5-7-10(9)12(8)3;/h4-7H,1-3H3;1H/q+1;/p-1" inchikey="RDSICPYJALLFAN-UHFFFAOYSA-M" height="200px" width="300px" float="none"> | |||
-INDIGO-05152410312D | |||
0 0 0 0 0 0 0 0 0 0 0 V3000 | |||
M V30 BEGIN CTAB | |||
M V30 COUNTS 13 13 0 0 0 | |||
M V30 BEGIN ATOM | |||
M V30 1 C 4.90985 -3.80007 0.0 0 | |||
M V30 2 C 6.64015 -3.79959 0.0 0 | |||
M V30 3 C 5.77664 -3.29997 0.0 0 | |||
M V30 4 C 6.64015 -4.80053 0.0 0 | |||
M V30 5 C 4.90985 -4.80502 0.0 0 | |||
M V30 6 C 5.77882 -5.30003 0.0 0 | |||
M V30 7 N 7.59213 -3.49022 0.0 0 CHG=1 | |||
M V30 8 C 8.18049 -4.29999 0.0 0 | |||
M V30 9 N 7.59212 -5.1098 0.0 0 | |||
M V30 10 C 8.09213 -2.62419 0.0 0 | |||
M V30 11 C 7.85094 -6.07572 0.0 0 | |||
M V30 12 C 9.18049 -4.29998 0.0 0 | |||
M V30 13 I 9.25 -3.225 0.0 0 CHG=-1 | |||
M V30 END ATOM | |||
M V30 BEGIN BOND | |||
M V30 1 2 3 1 | |||
M V30 2 2 4 2 | |||
M V30 3 1 1 5 | |||
M V30 4 1 2 3 | |||
M V30 5 2 5 6 | |||
M V30 6 1 6 4 | |||
M V30 7 1 2 7 | |||
M V30 8 2 7 8 | |||
M V30 9 1 8 9 | |||
M V30 10 1 9 4 | |||
M V30 11 1 7 10 | |||
M V30 12 1 9 11 | |||
M V30 13 1 8 12 | |||
M V30 END BOND | |||
M V30 END CTAB | |||
M END | |||
</chemform> | |||
====Photosensitizer==== | ====Photosensitizer==== | ||
<chemform smiles="N(C1C=CC=CC=1)1C2C=CC(N(C)C)=CC=2C2C=C(N(C)C)C=CC1=2" inchi="1S/C22H23N3/c1-23(2)17-10-12-21-19(14-17)20-15-18(24(3)4)11-13-22(20)25(21)16-8-6-5-7-9-16/h5-15H,1-4H3" inchikey="SEAGXMGVRJVEBS-UHFFFAOYSA-N" height="200px" width="300px" float="none"> | <chemform smiles="N(C1C=CC=CC=1)1C2C=CC(N(C)C)=CC=2C2C=C(N(C)C)C=CC1=2" inchi="1S/C22H23N3/c1-23(2)17-10-12-21-19(14-17)20-15-18(24(3)4)11-13-22(20)25(21)16-8-6-5-7-9-16/h5-15H,1-4H3" inchikey="SEAGXMGVRJVEBS-UHFFFAOYSA-N" height="200px" width="300px" float="none"> |
Revision as of 09:34, 15 May 2024
Abstract
Summary
A photochemical reduction of CO2 to CO was shown using -missing link parameter- as catalyst in combination with the organic carbazole-based photosensitizer 3,6-bis(dimethylamino)-9-phenyl-9H-carbazole. Turnover numbers (TONs) of 6080 for the catalyst and 8820 for the photosensitizer and an exclusive selectivity for formic acid were reached in MeCN/H2O with catalyst xx. The experiments were conducted under visible-light irradiation (λ = 400 nm) using ascorbic acid 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 HCOO- under visible-light catalysis using as a catalyst. The catalytic system performs best (referring to the TON of formic acid production) in MeCN/H2O.
Catalyst
1,2,3-Trimethylbenzimidazolium iodide
Photosensitizer
3,6-bis(dimethylamino)-9-phenyl-9H-carbazole
Investigation
Sacrificial electron donor
In this study, the experiments were done with the sacrificial electron donor ascorbic acid L-ascorbate, sodium. The use of BIH was tested, but found to yield worse results.
Additives
In this study, potassium carbonate was added as a base.
Investigations
- photocatalytic CO2 conversion under different conditions (Molecular process, Photocatalytic CO2 conversion experiments)