Merging an organic TADF photosensitizer and a simple terpyridine–Fe(iii) complex for photocatalytic CO2 reduction: Difference between revisions

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DOI 10.1039/d0cc05047d
Authors Yanan Wang, Xue-Wang Gao, Junli Li, Duobin Chao,
Submitted 03.09.2020
Published online 2020
Licenses http://rsc.li/journals-terms-of-use,
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[[Category:Photocatalytic CO2 conversion to CO]][[Category:Publication]]
[[Category:Photocatalytic CO2 conversion to CO]][[Category:Publication]]
{{BaseTemplate}}
{{BaseTemplate}}
===Abstract===
====Summary====
The photochemical reduction of CO<sub>2</sub> to CO was shown using the iron complex {{#moleculelink:|link=GKZBKMSETZXTMT-UHFFFAOYSA-K|image=false|width=300|height=200}} in combination with the organic photosensitizer {{#moleculelink:|link=PRWATGACIORDEL-UHFFFAOYSA-N|image=false|width=300|height=200}}. Turnover numbers (TONs) of up to 2250 and a selectivity of 99.3% for CO were reached in DMF/H<sub>2</sub>O. The experiments were conducted under visible-light irradiation (λ > 420 nm) with TEA (see section SEDs below) as sacrificial electron donor.
====Advances and special progress====
The presented study contains the first example for the use of an organic thermally activated delayed fluorescence (TADF) compound as a photosensitizer in CO<sub>2</sub> reduction.
====Additional remarks====
===Content of the published article in detail===
The article contains results of a study for the reduction of CO<sub>2</sub> to CO using an iron complex and an organic TADF photosensitizer. The catalytic system performs best (referring to the TON of CO production) in DMF.
====Catalyst====
<chemform smiles="C1C=CN2~[Fe]3(~N4=CC=CC=C4C4C=C(C5C=CC(C)=CC=5)C=C(N=4~3)C=2C=1)(Cl)(Cl)Cl" inchi="1S/C22H17N3.3ClH.Fe/c1-16-8-10-17(11-9-16)18-14-21(19-6-2-4-12-23-19)25-22(15-18)20-7-3-5-13-24-20;;;;/h2-15H,1H3;3*1H;/q;;;;+3/p-3" inchikey="GKZBKMSETZXTMT-UHFFFAOYSA-K" height="200px" width="300px" float="none">
  -INDIGO-05102414152D
  0  0  0  0  0  0  0  0  0  0  0 V3000
M  V30 BEGIN CTAB
M  V30 COUNTS 29 34 0 0 0
M  V30 BEGIN ATOM
M  V30 1 C 4.65985 -6.82507 0.0 0
M  V30 2 C 6.39015 -6.82459 0.0 0
M  V30 3 C 5.52664 -6.32497 0.0 0
M  V30 4 N 6.39015 -7.82553 0.0 0
M  V30 5 C 4.65985 -7.83002 0.0 0
M  V30 6 C 5.52882 -8.32503 0.0 0
M  V30 7 C 7.25641 -6.32499 0.0 0
M  V30 8 C 8.12013 -4.82569 0.0 0
M  V30 9 C 7.25603 -5.32428 0.0 0
M  V30 10 C 8.98731 -5.32558 0.0 0
M  V30 11 N 8.12705 -6.82688 0.0 0
M  V30 12 C 8.98989 -6.32126 0.0 0
M  V30 13 C 9.85818 -6.81733 0.0 0
M  V30 14 C 11.5885 -6.81569 0.0 0
M  V30 15 C 10.7246 -6.31664 0.0 0
M  V30 16 C 11.5891 -7.81663 0.0 0
M  V30 17 N 9.85885 -7.82228 0.0 0
M  V30 18 C 10.7282 -8.31671 0.0 0
M  V30 19 C 8.11993 -3.82569 0.0 0
M  V30 20 C 7.25335 -2.32802 0.0 0
M  V30 21 C 7.25309 -3.32566 0.0 0
M  V30 22 C 8.11986 -1.82697 0.0 0
M  V30 23 C 8.9899 -3.32263 0.0 0
M  V30 24 C 8.98344 -2.32257 0.0 0
M  V30 25 C 8.11823 -0.826972 0.0 0
M  V30 26 Fe 8.1 -8.325 0.0 0
M  V30 27 Cl 7.175 -8.95 0.0 0
M  V30 28 Cl 8.125 -9.375 0.0 0
M  V30 29 Cl 9.025 -8.925 0.0 0
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 9 7
M  V30 9 2 10 8
M  V30 10 1 7 11
M  V30 11 1 8 9
M  V30 12 2 11 12
M  V30 13 1 12 10
M  V30 14 1 12 13
M  V30 15 2 15 13
M  V30 16 2 16 14
M  V30 17 1 13 17
M  V30 18 1 14 15
M  V30 19 2 17 18
M  V30 20 1 18 16
M  V30 21 1 8 19
M  V30 22 2 21 19
M  V30 23 2 22 20
M  V30 24 1 19 23
M  V30 25 1 20 21
M  V30 26 2 23 24
M  V30 27 1 24 22
M  V30 28 1 22 25
M  V30 29 1 27 26
M  V30 30 1 28 26
M  V30 31 1 26 29
M  V30 32 8 4 26
M  V30 33 8 26 11
M  V30 34 8 26 17
M  V30 END BOND
M  V30 END CTAB
M  END
</chemform>
====Photosensitizer====
<chemform smiles="" inchi="" inchikey="PRWATGACIORDEL-UHFFFAOYSA-N" height="200px" width="300px" float="none"></chemform>
====Investigation====
{{#experimentlist:|form=Photocatalytic_CO2_conversion_experiments|name=photocatalytic reduction of CO2 to CO|importFile=}}
====Sacrificial electron donor====
In this study, the experiments were done with the sacrificial electron donor TEA ({{#moleculelink:|link=ZMANZCXQSJIPKH-UHFFFAOYSA-N|image=false|width=300|height=200}}).
====Additives====
In this study, no additives were tested. Control experiments with other photosensitizers (Ru(bpy)<sub>3</sub>, Fluorescein and Eosin Y) and catalysts (FeCl<sub>3</sub>) were conducted.
{{Tags|tags=CO2 reduction, photocatalysis, visible-light photochemistry, iron catalyst, Fe(tpy-tol)Cl3, organic photosensitizer, 4CzIPN, TADF photosensitizer, carbon monoxide evolution, sacrificial electron donor, triethylamine, homogeneous catalysis, high turnover number, DMF solvent, sustainable chemistry}}

Latest revision as of 11:41, 21 November 2025


Abstract[edit | edit source]

Summary[edit | edit source]

The photochemical reduction of CO2 to CO was shown using the iron complex Fe(tpy-tol)Cl3 in combination with the organic photosensitizer 4CzIPN. Turnover numbers (TONs) of up to 2250 and a selectivity of 99.3% for CO were reached in DMF/H2O. The experiments were conducted under visible-light irradiation (λ > 420 nm) with TEA (see section SEDs below) as sacrificial electron donor.

Advances and special progress[edit | edit source]

The presented study contains the first example for the use of an organic thermally activated delayed fluorescence (TADF) compound as a photosensitizer in CO2 reduction.

Additional remarks[edit | edit source]

Content of the published article in detail[edit | edit source]

The article contains results of a study for the reduction of CO2 to CO using an iron complex and an organic TADF photosensitizer. The catalytic system performs best (referring to the TON of CO production) in DMF.

Catalyst[edit | edit source]

Fe(tpy-tol)Cl3

Photosensitizer[edit | edit source]

4CzIPN

Investigation[edit | edit source]

catcat conc [µM]PSPS conc [mM]e-De-D conc [M]solvent A...λexc [nm].TON CO.
1.

Fe(tpy-tol)Cl3

10

4CzIPN

0.05

TEA

0.28

DMF

420-6502250
2.

Fe(tpy-tol)Cl3

10

4CzIPN

0.01

TEA

0.28

DMF

420-650133
3.

Fe(tpy-tol)Cl3

10

4CzIPN

0.05

TEA

0.28

DMF

420-650244
4.

Fe(tpy-tol)Cl3

10

4CzIPN

0.1

TEA

0.28

DMF

420-650246
5.

FeCl3

10

4CzIPN

0.05

TEA

0.28

DMF

420-6506
6.

Fe(tpy-tol)Cl3

10

Ru(bpy)3

0.05

TEA

0.28

DMF

420-65017
7.

Fe(tpy-tol)Cl3

10

Fluorescein

0.05

TEA

0.28

DMF

420-6500
8.

Fe(tpy-tol)Cl3

10

Eosin Y

0.05

TEA

0.28

DMF

420-6500
Investigation-Name: photocatalytic reduction of CO2 to CO

Sacrificial electron donor[edit | edit source]

In this study, the experiments were done with the sacrificial electron donor TEA (TEA).

Additives[edit | edit source]

In this study, no additives were tested. Control experiments with other photosensitizers (Ru(bpy)3, Fluorescein and Eosin Y) and catalysts (FeCl3) were conducted.

Tags: CO2 reduction, photocatalysis, visible-light photochemistry, iron catalyst, Fe(tpy-tol)Cl3, organic photosensitizer, 4CzIPN, TADF photosensitizer, carbon monoxide evolution, sacrificial electron donor, triethylamine, homogeneous catalysis, high turnover number, DMF solvent, sustainable chemistry

Investigations

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