Metal-free reduction of CO2 to formate using a photochemical organohydride-catalyst recycling strategy: Difference between revisions
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====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 HCOO<sup>-</sup> under visible-light catalysis using {{#moleculelink:|link=RDSICPYJALLFAN-UHFFFAOYSA-M|image=false|width=300|height=200}} as a catalyst. The catalytic system performs best (referring to the TON of formic acid production) in MeCN/H<sub>2</sub>O. | The article contains results for the reduction of CO<sub>2</sub> to HCOO<sup>-</sup> under visible-light catalysis using {{#moleculelink:|link=RDSICPYJALLFAN-UHFFFAOYSA-M|image=false|width=300|height=200}} as a catalyst. The catalytic system performs best (referring to the TON of formic acid production) in MeCN/H<sub>2</sub>O with photosensitizer {{#moleculelink:|link=SEAGXMGVRJVEBS-UHFFFAOYSA-N|image=false|width=300|height=200}}. | ||
====Catalyst==== | ====Catalyst==== | ||
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M V30 27 1 20 24 | M V30 27 1 20 24 | ||
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M END | |||
</chemform><chemform smiles="N1C2C=CC(N(C)C)=CC=2C2C=C(N(C)C)C=CC1=2" inchi="1S/C16H19N3/c1-18(2)11-5-7-15-13(9-11)14-10-12(19(3)4)6-8-16(14)17-15/h5-10,17H,1-4H3" inchikey="WRRDGZBKMQHXGG-UHFFFAOYSA-N" height="200px" width="300px" float="none"> | |||
-INDIGO-05152410542D | |||
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M V30 14 N 4.57069 -9.09212 0.0 0 | |||
M V30 15 N -1.06425 -9.09612 0.0 0 | |||
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M V30 19 C 5.54796 -8.88013 0.0 0 | |||
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M V30 17 1 7 15 | |||
M V30 18 1 15 16 | |||
M V30 19 1 15 17 | |||
M V30 20 1 14 18 | |||
M V30 21 1 14 19 | |||
M V30 END BOND | |||
M V30 END CTAB | |||
M END | |||
</chemform><chemform smiles="N(C1C=CC=CC=1)1C2C=CC(N(C3C=CC=CC=3)C3C=CC=CC=3)=CC=2C2C=C(N(C3C=CC=CC=3)C3C=CC=CC=3)C=CC1=2" inchi="1S/C42H31N3/c1-6-16-32(17-7-1)43(33-18-8-2-9-19-33)37-26-28-41-39(30-37)40-31-38(27-29-42(40)45(41)36-24-14-5-15-25-36)44(34-20-10-3-11-21-34)35-22-12-4-13-23-35/h1-31H" inchikey="PJLYJWBAONHQFV-UHFFFAOYSA-N" height="200px" width="300px" float="none"> | |||
-INDIGO-05152410562D | |||
0 0 0 0 0 0 0 0 0 0 0 V3000 | |||
M V30 BEGIN CTAB | |||
M V30 COUNTS 45 52 0 0 0 | |||
M V30 BEGIN ATOM | |||
M V30 1 N 7.825 -4.88056 0.0 0 | |||
M V30 2 C 8.63399 -5.46835 0.0 0 | |||
M V30 3 C 8.32499 -6.41944 0.0 0 | |||
M V30 4 C 7.32501 -6.41944 0.0 0 | |||
M V30 5 C 7.01601 -5.46835 0.0 0 | |||
M V30 6 C 6.65742 -7.15987 0.0 0 | |||
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M V30 8 C 6.03365 -5.25981 0.0 0 | |||
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M V30 10 C 9.60928 -5.26167 0.0 0 | |||
M V30 11 C 10.2788 -6.00479 0.0 0 | |||
M V30 12 C 8.99721 -7.16553 0.0 0 | |||
M V30 13 C 9.97346 -6.95178 0.0 0 | |||
M V30 14 C 7.82537 -1.92579 0.0 0 | |||
M V30 15 C 8.69094 -3.42404 0.0 0 | |||
M V30 16 C 8.69187 -2.4264 0.0 0 | |||
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M V30 45 C 13.2983 -7.92518 0.0 0 | |||
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M V30 31 1 22 29 | |||
M V30 32 1 26 27 | |||
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M V30 49 1 25 44 | |||
M V30 50 1 41 42 | |||
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M V30 END BOND | M V30 END BOND | ||
M V30 END CTAB | M V30 END CTAB |
Revision as of 09:56, 15 May 2024
Abstract
Summary
A photochemical reduction of CO2 to formic acid was shown using 1,2,3-Trimethylbenzimidazolium iodide 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. The experiments were conducted under visible-light irradiation (λ = 400 nm) using ascorbic acid as sacrificial electron donor (see section SEDs below) and potassium carbonate as a base.
Advances and special progress
A transition-metal free process for the efficient photocatalytic reduction of CO2 to formic acid was described. The use of an organohydride catalyst allowed for a high selectivity for formate without noteworthy formation of H2 or CO.
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 1,2,3-Trimethylbenzimidazolium iodide as a catalyst. The catalytic system performs best (referring to the TON of formic acid production) in MeCN/H2O with photosensitizer 3,6-bis(dimethylamino)-9-phenyl-9H-carbazole.
Catalyst
1,2,3-Trimethylbenzimidazolium iodide
Photosensitizer
3,6-bis(dimethylamino)-9-phenyl-9H-carbazole 3,6-bis(dimethylamino)carbazole 3,6-Bis(diphenylamino)-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)