Photocatalytic CO2 Reduction Using a Robust Multifunctional Iridium Complex toward the Selective Formation of Formic Acid: Difference between revisions
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{{ | {{DOI|doi=10.1021/jacs.0c03097}} | ||
[[Category:Photocatalytic CO2 conversion to HCOOH]] | [[Category:Photocatalytic CO2 conversion to HCOOH]] | ||
{{BaseTemplate}} | {{BaseTemplate}} | ||
==== | ===Abstract=== | ||
{{# | ====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 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. | |||
==== Catalyst ==== | ====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 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==== | |||
<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"> | ||
-INDIGO-05172314302D | -INDIGO-05172314302D | ||
| Line 205: | Line 213: | ||
</chemform> | </chemform> | ||
==== | ====Investigation ==== | ||
{{#experimentlist: |form=Photocatalytic_CO2_conversion_experiments|name=Photocatalytic reduction of CO2, best TON}} | |||
{{#experimentlist:|form=Photocatalytic_CO2_conversion_experiments|name=Control experiments|importFile=}} | |||
==== Sacrificial electron donor ==== | ====Sacrificial Electron Donor==== | ||
In this study, the experiments were done with the sacrificial electron donor BIH ({{#moleculelink:|link=VDFIVJSRRJXMAU-UHFFFAOYSA-N|image=false|width=300|height=200}}), water ({{#moleculelink:|link=XLYOFNOQVPJJNP-UHFFFAOYSA-N|image=false|width=300|height=200}}) and triethanolamine ({{#moleculelink:|link=GSEJCLTVZPLZKY-UHFFFAOYSA-N|image=false|width=300|height=200}}). | |||
====Additives==== | |||
In this study, additional control experiments were conducted with Hg. | |||
__FORCETOC__[[Category:Publication]] | |||
Latest revision as of 10:37, 11 April 2024
Abstract[edit | edit source]
Summary[edit | edit source]
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[edit | edit source]
The authors have developed a multifunctional catalyst that allows for selective generation of formic acid without the need for an external photosensitizer.
Additional remarks[edit | edit source]
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[edit | edit source]
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[edit | edit source]
Investigation[edit | edit source]
| cat | cat conc [µM] | e-D | e-D conc [M] | solvent A | . | . | λexc [nm] | . | TON CO | TON H2 | TON HCOOH | . | |
|---|---|---|---|---|---|---|---|---|---|---|---|---|---|
| 1. | 0.02 | 0.2 | >400 | 470 | 15 | 2080 |
Investigation-Name: Photocatalytic reduction of CO2, best TON
| cat | cat conc [µM] | solvent A | . | . | . | additives | . | . | . | λexc [nm] | . | TON CO | TON H2 | TON HCOOH | . | |
|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|
| 1. | 0.02 | Hg | >400 | 69 | 0.9 | 291 | ||||||||||
| 2. | 0.02 | >400 | 62 | 0.8 | 323 | |||||||||||
| 3. | 0.02 | >400 | 3.9 | 0.9 | 188 | |||||||||||
| 4. | 0.02 | >400 | 57 | 5 | 115 |
Investigation-Name: Control experiments
Sacrificial Electron Donor[edit | edit source]
In this study, the experiments were done with the sacrificial electron donor BIH (BIH), water (H2O) and triethanolamine (TEOA).
Additives[edit | edit source]
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)
