An integrated Re(I) photocatalyst and sensitizer that activates the formation of formic acid from reduction of CO2: Difference between revisions
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===Abstract=== | |||
====Summary==== | |||
A photochemical reduction of CO<sub>2</sub> to CO was shown using the nickel complex {{#moleculelink:|link=SOBXSEUOEROXNJ-UHFFFAOYSA-L|image=false|width=300|height=200}} as catalyst in combination with the ruthenium-based photosensitizer {{#moleculelink:|link=SJFYGUKHUNLZTK-UHFFFAOYSA-L|image=false|width=300|height=200}}. Turnover numbers (TONs) over 700 and a selectivity of >99% for CO were reached in dimethylacetamide/water. The experiments were conducted under visible-light irradiation (λ = 450 nm) using BIH as sacrificial reductants (see section SEDs below). | |||
====Advances and special progress==== | |||
A nickel catalyst inspired by the CODH enzyme (carbon monoxide dehydrogenase) was employed for the photocatalytic reduction of CO<sub>2</sub> with the back then highest reported TON values among nickel complexes in systems with [Ru(bpy)<sub>3</sub>]<sup>2+</sup>. | |||
====Additional remarks==== | |||
The binding of CO<sub>2</sub> to the nickel(0) species was identified as the potential rate-determining step of the reduction. | |||
=== 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 a nickel complex as a catalyst. The catalytic system performs best (referring to the TON of CO production) in dimethylacetamide/water. | |||
=== Catalyst=== | === Catalyst=== | ||
<chemform smiles="C1C=C2C3C=CC=CN=3[Re+]([C-]#[O+])([C-]#[O+])3(N4C=CC=CC=4C4N3=CC=CC=4)N2=CC=1.S(C(F)(F)F)([O-])(=O)=O" inchi="1S/2C10H8N2.CHF3O3S.2CO.Re/c2*1-3-7-11-9(5-1)10-6-2-4-8-12-10;2-1(3,4)8(5,6)7;2*1-2;/h2*1-8H;(H,5,6,7);;;/q;;;;;+1/p-1" inchikey="SQEHJZNRDJMTCB-UHFFFAOYSA-M" height="200px" width="300px" float="none"> | <chemform smiles="C1C=C2C3C=CC=CN=3[Re+]([C-]#[O+])([C-]#[O+])3(N4C=CC=CC=4C4N3=CC=CC=4)N2=CC=1.S(C(F)(F)F)([O-])(=O)=O" inchi="1S/2C10H8N2.CHF3O3S.2CO.Re/c2*1-3-7-11-9(5-1)10-6-2-4-8-12-10;2-1(3,4)8(5,6)7;2*1-2;/h2*1-8H;(H,5,6,7);;;/q;;;;;+1/p-1" inchikey="SQEHJZNRDJMTCB-UHFFFAOYSA-M" height="200px" width="300px" float="none"> | ||
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===Investigation=== | ===Investigation=== | ||
{{#experimentlist:|form=Photocatalytic_CO2_conversion_experiments|name=Table 1}} | {{#experimentlist:|form=Photocatalytic_CO2_conversion_experiments|name=Table 1}} | ||
====Sacrificial electron donor==== | |||
=== Sacrificial electron donor=== | In this study, the experiments were done with the sacrificial electron donor TEOA ([[Molecule:100507|100507]]). | ||
====Additives==== | |||
In this study, no additives were tested. | |||
Revision as of 10:27, 11 January 2024
Abstract
Summary
A photochemical reduction of CO2 to CO was shown using the nickel complex [Ni(bpet)(MeCN)2][ClO4]2 as catalyst in combination with the ruthenium-based photosensitizer Ru(bpy)3Cl2. Turnover numbers (TONs) over 700 and a selectivity of >99% for CO were reached in dimethylacetamide/water. The experiments were conducted under visible-light irradiation (λ = 450 nm) using BIH as sacrificial reductants (see section SEDs below).
Advances and special progress
A nickel catalyst inspired by the CODH enzyme (carbon monoxide dehydrogenase) was employed for the photocatalytic reduction of CO2 with the back then highest reported TON values among nickel complexes in systems with [Ru(bpy)3]2+.
Additional remarks
The binding of CO2 to the nickel(0) species was identified as the potential rate-determining step of the reduction.
Content of the published article in detail
The article contains results for the reduction of CO2 to CO under visible-light catalysis using a nickel complex as a catalyst. The catalytic system performs best (referring to the TON of CO production) in dimethylacetamide/water.
Catalyst
Toller Artikel über das Molekül [Ru(bpy)3][PF6], das total tolle Dinge kann.
Photosensitizer
Investigation
Sacrificial electron donor
In this study, the experiments were done with the sacrificial electron donor TEOA (100507).
Additives
In this study, no additives were tested.
Investigations
- Effect of proton donor (Molecular process, Photocatalytic CO2 conversion experiments)
- Solvent effect study between DMA DMF and acetonitrile (Molecular process, Photocatalytic CO2 conversion experiments)
- Study on the concentration of catalyst (Molecular process, Photocatalytic CO2 conversion experiments)
- Time profile in DMF (Molecular process, Photocatalytic CO2 conversion experiments)
