Photocatalytic CO2 Reduction Mediated by Electron Transfer via the Excited Triplet State of Zn(II) Porphyrin: Difference between revisions
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{{DOI|doi=10.1021/jacs.9b12712}} | {{DOI|doi=10.1021/jacs.9b12712}} | ||
[[Category:Photocatalytic CO2 conversion to CO]][[Category:Publication]] | [[Category:Photocatalytic CO2 conversion to CO]] | ||
[[Category:Publication]] | |||
{{BaseTemplate}} | {{BaseTemplate}} | ||
===Abstract=== | ===Abstract=== | ||
====Summary==== | ====Summary==== | ||
A photochemical reduction of CO<sub>2</sub> to CO was shown using the zinc porphyrin dyad with a connected rhenium complex {{#moleculelink:|link=|image=|width=|height=}} as a combined catalyst and photosensitizer molecule. Turnover numbers (TONs) of >1300 and a selectivity of >99.9% for CO were reached in DMA | A photochemical reduction of CO<sub>2</sub> to CO was shown using the zinc porphyrin dyad with a connected rhenium complex {{#moleculelink:|link=LYVLANYMDXKDOV-CVVGJFHCSA-M|image=false|width=300|height=200}} as a combined catalyst and photosensitizer molecule. Turnover numbers (TONs) of >1300 and a selectivity of >99.9% for CO were reached in DMA. The experiments were conducted under visible-light irradiation (λ = 420 nm) using BIH as sacrificial electron donor (see section SEDs below). | ||
====Advances and special progress==== | ====Advances and special progress==== | ||
A selective method for the reduction of CO<sub>2</sub> to CO with a porphyrin-rhenium complex dyad was presented, effectively linking the catalyst and photosensitizer in one molecule. | |||
====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 CO under visible-light catalysis using | The article contains results for the reduction of CO<sub>2</sub> to CO under visible-light catalysis using {{#moleculelink:|link=LYVLANYMDXKDOV-CVVGJFHCSA-M|image=false|width=300|height=200}} as a catalyst and photosensitizer. The catalytic system performs best (referring to the TON of CO production) in DMA. | ||
====Catalyst and Photosensitizer==== | ====Catalyst and Photosensitizer==== | ||
<chemform smiles="C1C2=C(C3C=CC(C(C)(C)C)=CC=3)C3N4[Zn]56~N7=C(C(C8C=CC9C=CC%10C=CC=N%11~[Re](~[C-]#[O+])(~[C-]#[O+])(~[C-]#[O+])(Br)~N=8C=9C=%10%11)=C8N5C(=C(C5C=CC(C(C)(C)C)=CC=5)C(=N2~6)C=1)C=C8)C=CC7=C(C1C=CC(C(C)(C)C)=CC=1)C4=CC=3" inchi="1S/C62H54N6.3CO.BrH.Re.Zn/c1-60(2,3)42-21-14-37(15-22-42)54-45-28-30-47(64-45)55(38-16-23-43(24-17-38)61(4,5)6)49-32-34-51(66-49)57(53-27-20-41-13-12-40-11-10-36-63-58(40)59(41)68-53)52-35-33-50(67-52)56(48-31-29-46(54)65-48)39-18-25-44(26-19-39)62(7,8)9;3*1-2;;;/h10-36H,1-9H3;;;;1H;;/q-2;;;;;+1;+2/p-1/b54-45-,54-46-,55-47-,55-49-,56-48-,56-50-,57-51+,57-52+;;;;;;" inchikey="LYVLANYMDXKDOV-CVVGJFHCSA-M" height="200px" width="300px" float="none"> | <chemform smiles="C1C2=C(C3C=CC(C(C)(C)C)=CC=3)C3N4[Zn]56~N7=C(C(C8C=CC9C=CC%10C=CC=N%11~[Re](~[C-]#[O+])(~[C-]#[O+])(~[C-]#[O+])(Br)~N=8C=9C=%10%11)=C8N5C(=C(C5C=CC(C(C)(C)C)=CC=5)C(=N2~6)C=1)C=C8)C=CC7=C(C1C=CC(C(C)(C)C)=CC=1)C4=CC=3" inchi="1S/C62H54N6.3CO.BrH.Re.Zn/c1-60(2,3)42-21-14-37(15-22-42)54-45-28-30-47(64-45)55(38-16-23-43(24-17-38)61(4,5)6)49-32-34-51(66-49)57(53-27-20-41-13-12-40-11-10-36-63-58(40)59(41)68-53)52-35-33-50(67-52)56(48-31-29-46(54)65-48)39-18-25-44(26-19-39)62(7,8)9;3*1-2;;;/h10-36H,1-9H3;;;;1H;;/q-2;;;;;+1;+2/p-1/b54-45-,54-46-,55-47-,55-49-,56-48-,56-50-,57-51+,57-52+;;;;;;" inchikey="LYVLANYMDXKDOV-CVVGJFHCSA-M" height="200px" width="300px" float="none"> | ||
| Line 192: | Line 195: | ||
</chemform> | </chemform> | ||
====Investigation==== | ====Investigation==== | ||
{{#experimentlist:|form=Photocatalytic_CO2_conversion_experiments|name=photocatalytic CO2 conversion|importFile=}} | |||
====Sacrificial electron donor==== | ====Sacrificial electron donor==== | ||
In this study, the experiments were done with the sacrificial electron donor | In this study, the experiments were done with the sacrificial electron donor {{#moleculelink:|link=VDFIVJSRRJXMAU-UHFFFAOYSA-N|image=false|width=300|height=200}}. | ||
====Additives==== | ====Additives==== | ||
In this study, | In this study, {{#moleculelink:|link=ISWSIDIOOBJBQZ-UHFFFAOYSA-N|image=false|width=300|height=200}} was used as an additive. | ||
Latest revision as of 15:59, 21 May 2024
Abstract[edit | edit source]
Summary[edit | edit source]
A photochemical reduction of CO2 to CO was shown using the zinc porphyrin dyad with a connected rhenium complex (Zn(tBuPP))-(Re(Phen)Br(CO)3) as a combined catalyst and photosensitizer molecule. Turnover numbers (TONs) of >1300 and a selectivity of >99.9% for CO were reached in DMA. The experiments were conducted under visible-light irradiation (λ = 420 nm) using BIH as sacrificial electron donor (see section SEDs below).
Advances and special progress[edit | edit source]
A selective method for the reduction of CO2 to CO with a porphyrin-rhenium complex dyad was presented, effectively linking the catalyst and photosensitizer in one molecule.
Additional remarks[edit | edit source]
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 (Zn(tBuPP))-(Re(Phen)Br(CO)3) as a catalyst and photosensitizer. The catalytic system performs best (referring to the TON of CO production) in DMA.
Catalyst and Photosensitizer[edit | edit source]
Investigation[edit | edit source]
| cat | cat conc [µM] | e-D | e-D conc [M] | solvent A | additives | . | . | λexc [nm] | . | TON CO | . | . | . | . | |
|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|
| 1. | 0.05 | 0.05 | phenol | 420 nm | 910 | ||||||||||
| 2. | 0.075 | 0.05 | phenol | 420 nm | 1340 | ||||||||||
| 3. | 0.05 | 0.05 | 420 nm | 520 |
Investigation-Name: photocatalytic CO2 conversion
Sacrificial electron donor[edit | edit source]
In this study, the experiments were done with the sacrificial electron donor BIH.
Additives[edit | edit source]
In this study, PhOH was used as an additive.
Investigations
- photocatalytic CO2 conversion (Molecular process, Photocatalytic CO2 conversion experiments)
