Water-Assisted Highly Efficient Photocatalytic Reduction of CO2 to CO with Noble Metal-Free Bis(terpyridine)iron(II) Complexes and an Organic Photosensitizer: Difference between revisions

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A photochemical reduction of CO<sub>2</sub> to CO was shown using the iron complexes {{#moleculelink: |link=VCSOHGDMTDAXCJ-UHFFFAOYSA-N|image=false|width=300|height=200}}, {{#moleculelink: |link=GNLSTNFUDXOKCD-UHFFFAOYSA-N|image=false|width=300|height=200}} and {{#moleculelink: |link=DJDQCCRAAYOAPK-UHFFFAOYSA-N|image=false|width=300|height=200}} as catalysts in combination with the organic photosensitizer {{#moleculelink:|link=PRWATGACIORDEL-UHFFFAOYSA-N|image=false|width=300|height=200}}. Turnover numbers (TONs) of 6320 and a selectivity of 99.4% for CO were reached in DMF/H<sub>2</sub>O with catalyst {{#moleculelink: |link=DJDQCCRAAYOAPK-UHFFFAOYSA-N|image=false|width=300|height=200}}. The experiments were conducted under visible-light irradiation (λ = 440 nm) using TEA as sacrificial electron donor (see section SEDs below).  
A photochemical reduction of CO<sub>2</sub> to CO was shown using the iron complexes {{#moleculelink: |link=VCSOHGDMTDAXCJ-UHFFFAOYSA-N|image=false|width=300|height=200}}, {{#moleculelink: |link=GNLSTNFUDXOKCD-UHFFFAOYSA-N|image=false|width=300|height=200}} and {{#moleculelink: |link=DJDQCCRAAYOAPK-UHFFFAOYSA-N|image=false|width=300|height=200}} as catalysts in combination with the organic photosensitizer {{#moleculelink:|link=PRWATGACIORDEL-UHFFFAOYSA-N|image=false|width=300|height=200}}. Turnover numbers (TONs) of 6320 and a selectivity of 99.4% for CO were reached in DMF/H<sub>2</sub>O with catalyst {{#moleculelink: |link=DJDQCCRAAYOAPK-UHFFFAOYSA-N|image=false|width=300|height=200}}. The experiments were conducted under visible-light irradiation (λ = 440 nm) using TEA as sacrificial electron donor (see section SEDs below).  
====Advances and special progress====
====Advances and special progress====
One of the highest TONs for CO<sub>2</sub> reduction with an organic thermally activated delayed fluorescence (TADF) compound as a photosensitizer was reported herein.
====Additional remarks====
====Additional remarks====
The addition of water was found to strongly promote the catalytic reaction.
===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 iron complex as a catalyst. The catalytic system performs best (referring to the TON of CO production) in DMF/H<sub>2</sub>O.
The article contains results for the reduction of CO<sub>2</sub> to CO under visible-light catalysis using the iron complex {{#moleculelink:|link=DJDQCCRAAYOAPK-UHFFFAOYSA-N|image=false|width=300|height=200}} as a catalyst. The catalytic system performs best (referring to the TON of CO production) in DMF/H<sub>2</sub>O.
====Catalyst====
====Catalyst====
<chemform smiles="C1C=CN2~[Fe]34(~N5C=CC=CC=5C5N~3=C(C=C(C3C=CC([*])=CC=3)C=5)C3C=CC=CN=3~4)3~N4=CC=CC=C4C4C=C(C5C=CC([*])=CC=5)C=C(N=4~3)C=2C=1" inchi="" inchikey="" height="200px" width="300px" float="none" r1="H,Cl,NMe2">
<chemform smiles="C1C=CN2~[Fe]34(~N5C=CC=CC=5C5N~3=C(C=C(C3C=CC([*])=CC=3)C=5)C3C=CC=CN=3~4)3~N4=CC=CC=C4C4C=C(C5C=CC([*])=CC=5)C=C(N=4~3)C=2C=1" inchi="" inchikey="" height="200px" width="300px" float="none" r1="H,Cl,NMe2">

Revision as of 08:54, 15 May 2024


Abstract

Summary

A photochemical reduction of CO2 to CO was shown using the iron complexes 100947, 100948 and 100949 as catalysts in combination with the organic photosensitizer 4CzIPN. Turnover numbers (TONs) of 6320 and a selectivity of 99.4% for CO were reached in DMF/H2O with catalyst 100949. The experiments were conducted under visible-light irradiation (λ = 440 nm) using TEA as sacrificial electron donor (see section SEDs below).

Advances and special progress

One of the highest TONs for CO2 reduction with an organic thermally activated delayed fluorescence (TADF) compound as a photosensitizer was reported herein.

Additional remarks

The addition of water was found to strongly promote the catalytic reaction.

Content of the published article in detail

The article contains results for the reduction of CO2 to CO under visible-light catalysis using the iron complex 100949 as a catalyst. The catalytic system performs best (referring to the TON of CO production) in DMF/H2O.

Catalyst

100946 [Show R-Groups]

Photosensitizer

4CzIPN

Investigation

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

Molecule:100949

0.01

4CzIPN

0.05

TEA

0.28

DMF

420-6506320
2.

Molecule:100948

0.01

4CzIPN

0.05

TEA

0.28

DMF

420-6502780
3.

Molecule:100947

0.01

4CzIPN

0.05

TEA

0.28

DMF

420-6504500
4.

Molecule:100949

0.01

Ru(bpy)3

0.05

TEA

0.28

DMF

420-65019
5.

Molecule:100949

0.01

4CzIPN

0.05

TEA

0.28

MeCN

420-650992
Investigation-Name: photocatalytic CO2 conversion

Sacrificial electron donor

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

Additives

In this study, no additives were tested.

Investigations