Photocatalytic CO2 Reduction Using a Robust Multifunctional Iridium Complex toward the Selective Formation of Formic Acid: Difference between revisions
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===Abstract=== | ===Abstract=== | ||
====Summary==== | ====Summary==== | ||
A photochemical reduction of CO<sub>2</sub> to formic acid and CO was shown using the iridium complex {{#moleculelink:|link=BEUJVGCRFICSDD-UHFFFAOYSA-M|image=false|width=300|height=200}} as a catalyst without any additional photosensitizer. Turnover numbers (TONs) of 2080 | A photochemical reduction of CO<sub>2</sub> to formic acid and CO was shown using the iridium complex {{#moleculelink:|link=BEUJVGCRFICSDD-UHFFFAOYSA-M|image=false|width=300|height=200}} as a catalyst without any additional photosensitizer. Turnover numbers (TONs) of 2080 and a selectivity of 87% for formic acid were reached in dimethylacetamide/water. The experiments were conducted under visible-light irradiation (λ > 400 nm) using BIH as sacrificial electron donor (see section SEDs below). | ||
==== Advances and special progress ==== | ==== Advances and special progress ==== | ||
The authors have developed a multifunctional catalyst that allows for selective generation of formic acid without the need for an external photosensitizer. | |||
====Additional remarks ==== | ====Additional remarks ==== | ||
The developed catalyst reduces CO2 to CO via inner-sphere catalysis and to formic acid via outer-sphere catalysis. | |||
===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 and formic acid under visible-light catalysis using an iridium complex. The catalytic system performs best (referring to the TON of formic acid production) in dimethylacetamide. | The article contains results for the reduction of CO<sub>2</sub> to CO and formic acid under visible-light catalysis using an iridium complex. The catalytic system performs best (referring to the TON of formic acid production) in dimethylacetamide/water. | ||
====Catalyst==== | ====Catalyst==== | ||
<chemform smiles="C(C1C(C)=CC(C)=CC=1C)1C=C2CP([Ir+3]([H-])([Cl-])34P(C5CCCCC5)(C5CCCCC5)CC5C=C(C6C(C)=CC(C)=CC=6C)C=C(C(C=1)=N23)N=54)(C1CCCCC1)C1CCCCC1.[B-](C1C=CC=CC=1)(C1C=CC=CC=1)(C1C=CC=CC=1)C1C=CC=CC=1" inchi="1S/C54H74N2P2.C24H20B.ClH.Ir.H/c1-37-27-39(3)53(40(4)28-37)43-31-45(35-57(47-19-11-7-12-20-47)48-21-13-8-14-22-48)55-51(33-43)52-34-44(54-41(5)29-38(2)30-42(54)6)32-46(56-52)36-58(49-23-15-9-16-24-49)50-25-17-10-18-26-50;1-5-13-21(14-6-1)25(22-15-7-2-8-16-22,23-17-9-3-10-18-23)24-19-11-4-12-20-24;;;/h27-34,47-50H,7-26,35-36H2,1-6H3;1-20H;1H;;/q;-1;;+3;-1/p-1" inchikey="BEUJVGCRFICSDD-UHFFFAOYSA-M" height="200px" width="300px" float="none"> | <chemform smiles="C(C1C(C)=CC(C)=CC=1C)1C=C2CP([Ir+3]([H-])([Cl-])34P(C5CCCCC5)(C5CCCCC5)CC5C=C(C6C(C)=CC(C)=CC=6C)C=C(C(C=1)=N23)N=54)(C1CCCCC1)C1CCCCC1.[B-](C1C=CC=CC=1)(C1C=CC=CC=1)(C1C=CC=CC=1)C1C=CC=CC=1" inchi="1S/C54H74N2P2.C24H20B.ClH.Ir.H/c1-37-27-39(3)53(40(4)28-37)43-31-45(35-57(47-19-11-7-12-20-47)48-21-13-8-14-22-48)55-51(33-43)52-34-44(54-41(5)29-38(2)30-42(54)6)32-46(56-52)36-58(49-23-15-9-16-24-49)50-25-17-10-18-26-50;1-5-13-21(14-6-1)25(22-15-7-2-8-16-22,23-17-9-3-10-18-23)24-19-11-4-12-20-24;;;/h27-34,47-50H,7-26,35-36H2,1-6H3;1-20H;1H;;/q;-1;;+3;-1/p-1" inchikey="BEUJVGCRFICSDD-UHFFFAOYSA-M" height="200px" width="300px" float="none"> |
Revision as of 16:16, 22 January 2024
Abstract
Summary
A photochemical reduction of CO2 to formic acid and CO was shown using the iridium complex [Ir(mesbpy-(PCy2)2)][BPh4] as a catalyst without any additional photosensitizer. Turnover numbers (TONs) of 2080 and a selectivity of 87% for formic acid were reached in dimethylacetamide/water. The experiments were conducted under visible-light irradiation (λ > 400 nm) using BIH as sacrificial electron donor (see section SEDs below).
Advances and special progress
The authors have developed a multifunctional catalyst that allows for selective generation of formic acid without the need for an external photosensitizer.
Additional remarks
The developed catalyst reduces CO2 to CO via inner-sphere catalysis and to formic acid via outer-sphere catalysis.
Content of the published article in detail
The article contains results for the reduction of CO2 to CO and formic acid under visible-light catalysis using an iridium complex. The catalytic system performs best (referring to the TON of formic acid production) in dimethylacetamide/water.
Catalyst
Investigation
Sacrificial Electron Donor
In this study, the experiments were done with the sacrificial electron donor BIH (BIH).
Additives
In this study, additional control experiments were conducted with Hg.
Investigations
- Control experiments (Molecular process, Photocatalytic CO2 conversion experiments)
- Photocatalytic reduction of CO2, best TON (Molecular process, Photocatalytic CO2 conversion experiments)