Photocatalytic Reduction of CO2 by Highly Efficient Homogeneous FeII Catalyst based on 2,6-Bis(1’,2’,3’-triazolyl-methyl)pyridine. Comparison with Analogues.: Difference between revisions

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===Abstract===
===Abstract===
====Summary====
====Summary====
A photochemical reduction of CO<sub>2</sub> to CO was shown using the iron complex {{#moleculelink:|link=ZCGUPOIZKSBSCM-UHFFFAOYSA-N|image=false|width=300|height=200}} as catalyst in combination with the copper photosensitizer {{#moleculelink:|link=SVWABAAUBHILMW-UHFFFAOYSA-P|image=false|width=300|height=200}}. Turnover numbers (TONs) of 576 and a selectivity of 67% for CO were reached in MeCN/TEOA. The experiments were conducted under visible-light irradiation (λ = 420 nm) using BIH as sacrificial electron donor (see section SEDs below). The homoleptic iron complex and the cobalt complexes and were tested for CO<sub>2</sub> reduction as well, but did not show substantial conversion of CO<sub>2</sub> to CO.  
A photochemical reduction of CO<sub>2</sub> to CO was shown using the iron complex {{#moleculelink:|link=ZCGUPOIZKSBSCM-UHFFFAOYSA-N|image=false|width=300|height=200}} as catalyst in combination with the copper photosensitizer {{#moleculelink:|link=SVWABAAUBHILMW-UHFFFAOYSA-P|image=false|width=300|height=200}}. Turnover numbers (TONs) of 576 and a selectivity of 67% for CO were reached in MeCN/TEOA. The experiments were conducted under visible-light irradiation (λ = 420 nm) using BIH as sacrificial electron donor (see section SEDs below). The homoleptic iron complex {{#moleculelink:|link=SIMPDUKIPFZEDX-UHFFFAOYSA-N|image=false|width=300|height=200}} and the cobalt complexes {{#moleculelink:|link=JDMNOCVBLMVSON-UHFFFAOYSA-N|image=false|width=300|height=200}} and {{#moleculelink:|link=QMZVNZOKJUBNLZ-UHFFFAOYSA-N|image=false|width=300|height=200}} were tested for CO<sub>2</sub> reduction as well, but did not show substantial conversion of CO<sub>2</sub> to CO.  
====Advances and special progress====
====Advances and special progress====
The authors reported a iron complex with one of the highest activities for CO<sub>2</sub> reduction among earth-abundant systems with monometallic iron catalysts.
The authors reported a iron complex with one of the highest activities for CO<sub>2</sub> reduction among earth-abundant systems with monometallic iron catalysts.
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Line 259: Line 658:


====Investigation====
====Investigation====
{{#experimentlist: |form=Photocatalytic_CO2_conversion_experiments|name=Optimization of CO2 reduction conditions|importFile=}}
{{#experimentlist:|form=Photocatalytic_CO2_conversion_experiments|name=CO2 reduction experiments testing different catalysts|importFile=}}
====Sacrificial electron donor====
====Sacrificial electron donor====
In this study, the experiments were done with the sacrificial electron donor BIH ([[Molecule:100508|100508]]).
In this study, the experiments were done with the sacrificial electron donor BIH ([[Molecule:100508|100508]]).
====Additives====
====Additives====
In this study, control experiments with Hg and without CO<sub>2</sub> were conducted.
In this study, control experiments with Hg and without CO<sub>2</sub> were conducted.

Latest revision as of 14:03, 16 May 2024


Abstract[edit | edit source]

Summary[edit | edit source]

A photochemical reduction of CO2 to CO was shown using the iron complex 100941 as catalyst in combination with the copper photosensitizer 100940. Turnover numbers (TONs) of 576 and a selectivity of 67% for CO were reached in MeCN/TEOA. The experiments were conducted under visible-light irradiation (λ = 420 nm) using BIH as sacrificial electron donor (see section SEDs below). The homoleptic iron complex 100942 and the cobalt complexes 100944 and 100945 were tested for CO2 reduction as well, but did not show substantial conversion of CO2 to CO.

Advances and special progress[edit | edit source]

The authors reported a iron complex with one of the highest activities for CO2 reduction among earth-abundant systems with monometallic iron catalysts.

Additional remarks[edit | edit source]

In addition to the production of CO, a substantial amount of H2 (TON of 287) was formed in the reduction process with complex 100941.

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

The article contains results for the reduction of CO2 to CO under visible-light catalysis using the iron complex 100941 as a catalyst. The catalytic system performs best (referring to the TON of CO production) in MeCN/TEOA.

Catalyst[edit | edit source]

100941 100942 100944 100945

Photosensitizer[edit | edit source]

100940

Investigation[edit | edit source]

catcat conc [µM]PSPS conc [mM]e-De-D conc [M]solvent A..additives..λexc [nm].TON COTON CH4TON H2.
1.

Molecule:100941

0.1

Molecule:100940

1.0

BIH

0.02

MeCN

42010743
2.

Molecule:100941

0.1

Molecule:100940

1.0

BIH

0.02

MeCN

42010954
3.

Molecule:100941

0.03

Molecule:100940

0.33

BIH

0.00666

MeCN

420238137
4.

Molecule:100941

0.03

Molecule:100940

1.0

BIH

0.02

MeCN

420314151
5.

Molecule:100941

0.01

Molecule:100940

1.0

BIH

0.02

MeCN

420576287
6.

Molecule:100941

0.1

Molecule:100940

1.0

BIH

0.1

MeCN

4208033
7.

Molecule:100941

0.1

Molecule:100940

1.0

BIH

0.1

MeCN

water4207.46.4
8.

Molecule:100941

0.1

Molecule:100940

1.0

BIH

0.02

MeCN

4203.21.6
9.

Molecule:100941

0.1

Molecule:100940

1.0

BIH

0.02

MeCN

4208034
10.

Molecule:100941

0.1

Molecule:100940

1.0

BIH

0.02

MeCN

42010043
11.


Molecule:100940

1.0

BIH

0.02

MeCN

42001
12.

Molecule:100941

0.1


BIH

0.02

MeCN

42000
13.

Molecule:100941

0.1

Molecule:100940

1.0

BIH

0.02

MeCN

00
14.

Molecule:100941

0.1

Molecule:100940

1.0

BIH

0.02

MeCN

42000
15.

Molecule:100941

0.1

Molecule:100940

1.0

BIH

0.02

MeCN

Hg4209350
16.

Molecule:100941

0.1

Molecule:100940

1.0

BIH

0.02

MeCN

solar simulator450348
17.

Molecule:100941

0.01

Molecule:100940

1.0


MeCN

4206.800
18.

Molecule:100941

0.01

Molecule:100940

1.0

BIH

0.02

MeCN

420441.160
19.

Molecule:100941

0.01

Molecule:100940

1.0


MeCN

420000
20.

Molecule:100941

0.01

Molecule:100940

1.0

BIH

0.02

MeCN

420000
catcat conc [µM]PSPS conc [mM]e-De-D conc [M]solvent A...λexc [nm].TON COTON H2.
1.

Molecule:100942

0.1

Molecule:100940

1.0

BIH

0.02

MeCN

4207.82
2.

Molecule:100944

0.1

Molecule:100940

1.0

BIH

0.02

MeCN

4201.17.4
3.

Molecule:100945

0.1

Molecule:100940

1.0

BIH

0.02

MeCN

4200.74.9

Sacrificial electron donor[edit | edit source]

In this study, the experiments were done with the sacrificial electron donor BIH (100508).

Additives[edit | edit source]

In this study, control experiments with Hg and without CO2 were conducted.

Investigations