Photochemical Reduction of Carbon Dioxide to Formic Acid using Ruthenium(II)-Based Catalysts and Visible Light: Difference between revisions

Latest revision as of 15:15, 5 July 2024

A photochemical reduction of CO₂ to formic acid was shown using a system containing an iridium-based photosensitizer, ruthenium photocatalyst and triethanolamine as the electron donor. Turnover numbers up to 526 and a selectivity of 80% towards formic acid were observed if the reaction was performed with [Ir(ppy)₂(bpy)]PF₆ ([Ir(ppy)2(bpy)][PF6]) as the photosensitizer and [Ru(bpy)₂(Cl)(CO)]PF₆ (100837) as the catalyst. The experiments were conducted under irradiation with Hg-lamp equipped with a λ=400–700 nm filter.

Advances and special progress[edit | edit source]

The employed photocatalytic system showed activity for the photoreduction of Na₂CO₃ to formic acid as well. A TON of 53 was observed after 5h reaction time.

Additional remarks[edit | edit source]

Experiments using different electron and proton donors such as triethylamine (TEA) and 1-benzyl-1,4-dihydronicotinamide (BNAH) were unsuccessful as the observed activities were lower than those obtained in the presence of TEOA.

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

The article contains results for the reduction of CO2 to formic under visible-light catalysis using ruthenium complexes as catalysts, the iridium complex [Ir(ppy)₂(bpy)]PF₆ ([Ir(ppy)2(bpy)][PF6]) as a photosensitizer and triethanolamine as the electron donor. The catalytic system performs best (referring to the TON of HCOOH production) with [Ru(bpy)₂(Cl)(CO)]PF₆ (100837) as photocatalyst.

Catalysts[edit | edit source]

Ru(bpy)2Cl2 Ru(bpy)2CO3 [Ru(bpy)2ClCO][PF6] [Ru(bpy)(H2O)(CO)][PF6] [Ru(bpy)(AcMe)2][PF6] [Ru(bpy)2HCO][PF6]

Photosensitizer[edit | edit source]

[Ir(ppy)2(bpy)][PF6]

Investigations[edit | edit source]

	cat	cat conc [µM]	PS	PS conc [mM]	e-D	solvent A	λexc [nm]	TON CO	TON H2	TON HCOOH
1.	Ru(bpy)2Cl2	25	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	1	2	13
2.	Ru(bpy)2CO3	25	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	2	4	21
3.	[Ru(bpy)2ClCO][PF6]	25	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	13	8	62
4.	[Ru(bpy)2HCO][PF6]	25	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	8	8	34
5.	[Ru(bpy)(H2O)(CO)][PF6]	25	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	7	9	40
6.	[Ru(bpy)(AcMe)2][PF6]	25	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	3	4	27

Investigation-Name: CO2 reduction experiments

	cat	cat conc [µM]	PS	PS conc [mM]	e-D	solvent A	λexc [nm]	TON CO	TON H2	TON HCOOH
1.	Ru(bpy)2Cl2	6.2	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	3	9	26
2.	Ru(bpy)2CO3	6.2	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	3	11	39
3.	[Ru(bpy)2ClCO][PF6]	6.2	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	19	19	117
4.	[Ru(bpy)2HCO][PF6]	6.2	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	21	16	107
5.	[Ru(bpy)(H2O)(CO)][PF6]	6.2	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	21	14	75
6.	[Ru(bpy)(AcMe)2][PF6]	6.2	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	4	12	64
7.	[Ru(bpy)2ClCO][PF6]	3.1	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	36	33	296
8.	[Ru(bpy)2HCO][PF6]	3.1	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	16	29	145
9.	[Ru(bpy)(H2O)(CO)][PF6]	3.1	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	34	28	211
10.	[Ru(bpy)2ClCO][PF6]	1.6	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	40	67	419
11.	[Ru(bpy)2HCO][PF6]	1.6	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	25	62	225
12.	[Ru(bpy)(H2O)(CO)][PF6]	1.6	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	45	65	335
13.	[Ru(bpy)(AcMe)2][PF6]	1.6	[Ir(ppy)2(bpy)][PF6]	0.025	TEOA	NMP	400 - 700	4	44	75

Investigation-Name: Optimization of concentrations

	analyte	reduction potential	solvent	electrolyte	WE	RE
1.	Ru(bpy)2Cl2	0,-2.11	MeCN	TBABF4	glassy carbon	Ag/AgNO3 in MeCN
2.	Ru(bpy)2CO3	0.45,-1.97	MeCN	TBABF4	glassy carbon	Ag/AgNO3 in MeCN
3.	[Ru(bpy)2ClCO][PF6]	1.22,-1.75	MeCN	TBABF4	glassy carbon	Ag/AgNO3 in MeCN
4.	[Ru(bpy)2HCO][PF6]	1.20,-1.61	MeCN	TBABF4	glassy carbon	Ag/AgNO3 in MeCN

Investigation-Name: Table 3 - CV

Sacrificial electron donor[edit | edit source]

In this study, the experiments were done with the sacrificial electron donor TEOA (100507).

Additives[edit | edit source]

No additives were used in the described experiments.

Investigations

CO2 reduction experiments (Molecular process, Photocatalytic CO2 conversion experiments)
Optimization of concentrations (Molecular process, Photocatalytic CO2 conversion experiments)
Table 1 (Molecular process, Photocatalytic CO2 conversion experiments)
Table 2 (Molecular process, Photocatalytic CO2 conversion experiments)
Table 3 - CV (Assay, Cyclic Voltammetry experiments)

DOI	10.1002/cctc.201500494
Authors	Alonso Rosas-Hernández, Henrik Junge, Matthias Beller,
Submitted	26.08.2015
Published online	26.08.2015
Licenses	http://doi.wiley.com/10.1002/tdm_license_1.1,
Subjects	Inorganic Chemistry, Organic Chemistry, Physical and Theoretical Chemistry, Catalysis
Go to literature page

Photochemical Reduction of Carbon Dioxide to Formic Acid using Ruthenium(II)-Based Catalysts and Visible Light: Difference between revisions

Latest revision as of 15:15, 5 July 2024

Contents

Abstract[edit | edit source]

Summary[edit | edit source]

Advances and special progress[edit | edit source]

Additional remarks[edit | edit source]

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

Catalysts[edit | edit source]

Photosensitizer[edit | edit source]

Investigations[edit | edit source]

Sacrificial electron donor[edit | edit source]

Additives[edit | edit source]

Investigations

Topics

@@ Line 1: / Line 1: @@
 {{BaseTemplate}}
 [[Category:Photocatalytic CO2 conversion to HCOOH]]
-{{#doiinfobox: 10.1002/cctc.201500494 }}{{MissingInvestigation}}{{FaultyMolecule}}
+{{DOI|doi=10.1002/cctc.201500494 }}
 === Abstract ===
 ==== Summary ====
-A photochemical reduction of CO<sub>2</sub> to formic acid was shown using a system containing an iridium-based photosensitizer, ruthenium photocatalyst and triethanolamine as the electron donor. Turnover numbers up to 526 and a selectivity of 80% towards formic acid were observed if the reaction was performed with [Ir(ppy)<sub>2</sub>(bpy)]PF<sub>6</sub> ({{#moleculelink:|link=RJJGJTKSOSSNNL-UHFFFAOYSA-N|image=false|width=300|height=200}}) as the photosensitizer and [Ru(bpy)<sub>2</sub>(Cl)(CO)]PF<sub>6</sub> as the catalyst.  The experiments were conducted under irradiation with Hg-lamp equipped with a ''λ''=400–700 nm filter.
+A photochemical reduction of CO<sub>2</sub> to formic acid was shown using a system containing an iridium-based photosensitizer, ruthenium photocatalyst and triethanolamine as the electron donor. Turnover numbers up to 526 and a selectivity of 80% towards formic acid were observed if the reaction was performed with [Ir(ppy)<sub>2</sub>(bpy)]PF<sub>6</sub> ({{#moleculelink:|link=RJJGJTKSOSSNNL-UHFFFAOYSA-N|image=false|width=300|height=200}}) as the photosensitizer and [Ru(bpy)<sub>2</sub>(Cl)(CO)]PF<sub>6</sub> ({{#moleculelink: |link=WUXWMOMXGWJDBM-UHFFFAOYSA-M|image=false|width=300|height=200}}) as the catalyst.  The experiments were conducted under irradiation with Hg-lamp equipped with a ''λ''=400–700 nm filter.
 ==== Advances and special progress ====
@@ Line 15: / Line 14: @@
 === Content of the published article in detail ===
-The article contains results for the reduction of CO2 to formic under visible-light catalysis using ruthenium complexes as catalysts, the iridium complex [Ir(ppy)<sub>2</sub>(bpy)]PF<sub>6</sub> ({{#moleculelink:|link=RJJGJTKSOSSNNL-UHFFFAOYSA-N|image=false|width=300|height=200}}) as a photosensitizer and triethanolamine as the electron donor. The catalytic system performs best (referring to the TON of HCOOH production) with [Ru(bpy)<sub>2</sub>(Cl)(CO)]PF<sub>6</sub> as photocatalyst.
+The article contains results for the reduction of CO2 to formic under visible-light catalysis using ruthenium complexes as catalysts, the iridium complex [Ir(ppy)<sub>2</sub>(bpy)]PF<sub>6</sub> ({{#moleculelink:|link=RJJGJTKSOSSNNL-UHFFFAOYSA-N|image=false|width=300|height=200}}) as a photosensitizer and triethanolamine as the electron donor. The catalytic system performs best (referring to the TON of HCOOH production) with [Ru(bpy)<sub>2</sub>(Cl)(CO)]PF<sub>6</sub> ({{#moleculelink: |link=WUXWMOMXGWJDBM-UHFFFAOYSA-M|image=false|width=300|height=200}}) as photocatalyst.
 ==== Catalysts ====
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-M  V30 21 N 4.76515 -6.64959 0.0 0
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-M  V30 25 C 3.90382 -8.15003 0.0 0
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-M  V30 26 C 5.63166 -8.1497 0.0 0
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-M  V30 32 Ru 6.48118 -5.65053 0.0 0 CHG=2
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-M  V30 33 R# 7.4971 -4.94171 0.0 0 RGROUPS=(1 1)
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 M  V30 END ATOM
 M  V30 BEGIN BOND
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 M  V30 END BOND
 M  V30 END CTAB
 M  END
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   0  0  0  0  0  0  0  0  0  0 V3000
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 M  V30 BEGIN ATOM
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-M  V30 41 R# 8.88398 -4.525 0.0 0 RGROUPS=(1 1)
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 M  V30 END ATOM
 M  V30 BEGIN BOND
@@ Line 337: / Line 447: @@
 M  V30 37 2 37 38
 M  V30 38 1 38 36
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+M  V30 END BOND
+M  V30 END CTAB
+M  END
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+  -INDIGO-02262411182D
+  0  0  0  0  0  0  0  0  0  0 V3000
+M  V30 BEGIN CTAB
+M  V30 COUNTS 35 39 0 0 0
+M  V30 BEGIN ATOM
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 M  V30 END BOND
 M  V30 END CTAB
@@ Line 459: / Line 661: @@
 ==== Investigations ====
-{{#experimentlist:|form=Photocatalytic_CO2_conversion_experiments|name=Table 1}}
+{{#experimentlist: |form=Photocatalytic_CO2_conversion_experiments|name=CO2 reduction experiments}}
-{{#experimentlist:|form=Photocatalytic_CO2_conversion_experiments|name=Table 2}}
+{{#experimentlist: |form=Photocatalytic_CO2_conversion_experiments|name=Optimization of concentrations}}
 {{#experimentlist:|form=Cyclic_Voltammetry_experiments|name=Table 3 - CV}}
@@ Line 469: / Line 671: @@
 ==== Additives ====
-No additives were used in the described experiments.
+No additives were used in the described experiments.[[Category:Publication]]

Photochemical Reduction of Carbon Dioxide to Formic Acid using Ruthenium(II)-Based Catalysts and Visible Light: Difference between revisions

Latest revision as of 15:15, 5 July 2024

Abstract[edit | edit source]

Summary[edit | edit source]

Advances and special progress[edit | edit source]

Additional remarks[edit | edit source]

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

Catalysts[edit | edit source]

Photosensitizer[edit | edit source]

Investigations[edit | edit source]

Sacrificial electron donor[edit | edit source]

Additives[edit | edit source]

Investigations

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