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

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 [[Category:Photocatalytic CO2 conversion to HCOOH]]
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+M  V30 26 C 8.64809 -3.05737 0.0 0
-M  V30 27 C 4.76127 -6.39566 0.0 0
+M  V30 27 C 4.98697 -6.01514 0.0 0
-M  V30 28 N 6.24241 -6.39524 0.0 0
+M  V30 28 N 6.45845 -6.01473 0.0 0
-M  V30 29 C 5.50325 -5.96757 0.0 0
+M  V30 29 C 5.7241 -5.58984 0.0 0
-M  V30 30 C 6.24241 -7.25205 0.0 0
+M  V30 30 C 6.45845 -6.86595 0.0 0
-M  V30 31 C 4.76127 -7.2559 0.0 0
+M  V30 31 C 4.98697 -6.86977 0.0 0
-M  V30 32 C 5.50512 -7.67963 0.0 0
+M  V30 32 C 5.72596 -7.29074 0.0 0
-M  V30 33 C 6.98415 -7.67934 0.0 0
+M  V30 33 C 7.19535 -7.29046 0.0 0
-M  V30 34 C 8.46535 -7.67651 0.0 0
+M  V30 34 C 8.66688 -7.28764 0.0 0
-M  V30 35 N 7.72543 -7.25004 0.0 0
+M  V30 35 N 7.93179 -6.86395 0.0 0
-M  V30 36 C 8.46673 -8.53333 0.0 0
+M  V30 36 C 8.66826 -8.13887 0.0 0
-M  V30 37 C 6.98556 -8.53958 0.0 0
+M  V30 37 C 7.19675 -8.14508 0.0 0
-M  V30 38 C 7.73009 -8.96211 0.0 0
+M  V30 38 C 7.93643 -8.56485 0.0 0
-M  V30 39 Ru 7.70092 -5.43455 0.0 0
+M  V30 39 Ru 7.90744 -5.10948 0.0 0 CHG=2
-M  V30 40 O 9.09194 -4.53455 0.0 0
+M  V30 40 O 9.27558 -4.15054 0.0 0
-M  V30 41 O 9.14194 -6.10955 0.0 0
+M  V30 41 O 9.32346 -5.80948 0.0 0
-M  V30 42 C 9.95797 -4.03455 0.0 0
+M  V30 42 C 10.1416 -3.65054 0.0 0
-M  V30 43 C 10.1079 -6.36837 0.0 0
+M  V30 43 C 10.1416 -2.65054 0.0 0
-M  V30 44 C 9.95797 -3.03455 0.0 0
+M  V30 44 C 11.0076 -4.15054 0.0 0
-M  V30 45 C 10.824 -4.53455 0.0 0
+M  V30 45 C 10.1895 -6.30948 0.0 0
-M  V30 46 C 10.3667 -7.33429 0.0 0
+M  V30 46 C 11.0555 -5.80948 0.0 0
-M  V30 47 C 10.815 -5.66126 0.0 0
+M  V30 47 C 10.1895 -7.30948 0.0 0
 M  V30 END ATOM
 M  V30 BEGIN BOND
@@ Line 352: / Line 454: @@
 M  V30 44 10 39 41
 M  V30 45 2 40 42
-M  V30 46 2 41 43
+M  V30 46 1 42 43
 M  V30 47 1 42 44
-M  V30 48 1 42 45
+M  V30 48 2 41 45
-M  V30 49 1 43 46
+M  V30 49 1 45 46
-M  V30 50 1 43 47
+M  V30 50 1 45 47
+M  V30 END BOND
+M  V30 END CTAB
+M  END
+</chemform><chemform smiles="C1C=CN2[Ru+2]([C-]#[O+])([H-])3(N4C=CC=CC=4C4C=CC=CN=43)N3=CC=CC=C3C=2C=1.F[P-](F)(F)(F)(F)F" inchi="1S/2C10H8N2.CO.F6P.Ru.H/c2*1-3-7-11-9(5-1)10-6-2-4-8-12-10;1-2;1-7(2,3,4,5)6;;/h2*1-8H;;;;/q;;;-1;+2;-1" inchikey="HJTHNVDYVJWKQG-UHFFFAOYSA-N" height="200px" width="300px" float="none">
+  -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
+M  V30 1 C 4.57242 -3.91012 0.0 0
+M  V30 2 C 6.0439 -3.90972 0.0 0
+M  V30 3 C 5.30956 -3.48483 0.0 0
+M  V30 4 N 6.0439 -4.76094 0.0 0
+M  V30 5 C 4.57242 -4.76476 0.0 0
+M  V30 6 C 5.31141 -5.18573 0.0 0
+M  V30 7 C 6.78059 -3.48485 0.0 0
+M  V30 8 C 7.51572 -2.21015 0.0 0
+M  V30 9 C 6.78066 -2.63382 0.0 0
+M  V30 10 C 8.25303 -2.6356 0.0 0
+M  V30 11 N 7.52081 -3.91201 0.0 0
+M  V30 12 C 8.2548 -3.48237 0.0 0
+M  V30 13 C 4.59368 -6.44014 0.0 0
+M  V30 14 N 6.06516 -6.43973 0.0 0
+M  V30 15 C 5.33081 -6.01484 0.0 0
+M  V30 16 C 6.06516 -7.29095 0.0 0
+M  V30 17 C 4.59368 -7.29477 0.0 0
+M  V30 18 C 5.33267 -7.71574 0.0 0
+M  V30 19 C 6.80206 -7.71546 0.0 0
+M  V30 20 C 8.27359 -7.71264 0.0 0
+M  V30 21 N 7.5385 -7.28895 0.0 0
+M  V30 22 C 8.27497 -8.56387 0.0 0
+M  V30 23 C 6.80346 -8.57008 0.0 0
+M  V30 24 C 7.54314 -8.98985 0.0 0
+M  V30 25 Ru 7.51415 -5.53448 0.0 0 CHG=2
+M  V30 26 H 8.88229 -4.57554 0.0 0 CHG=-1
+M  V30 27 C 8.93149 -6.24753 0.0 0 CHG=-1
+M  V30 28 O 9.78318 -6.7393 0.0 0 CHG=1
+M  V30 29 F 10.5241 -4.07553 0.0 0
+M  V30 30 P 11.3758 -3.58377 0.0 0 CHG=-1
+M  V30 31 F 12.2276 -4.07553 0.0 0
+M  V30 32 F 11.3758 -2.60024 0.0 0
+M  V30 33 F 10.5241 -3.09201 0.0 0
+M  V30 34 F 12.2276 -3.09201 0.0 0
+M  V30 35 F 11.3758 -4.5673 0.0 0
+M  V30 END ATOM
+M  V30 BEGIN BOND
+M  V30 1 2 3 1
+M  V30 2 2 4 2
+M  V30 3 1 1 5
+M  V30 4 1 2 3
+M  V30 5 2 5 6
+M  V30 6 1 6 4
+M  V30 7 1 2 7
+M  V30 8 2 9 7
+M  V30 9 2 10 8
+M  V30 10 1 7 11
+M  V30 11 1 8 9
+M  V30 12 2 11 12
+M  V30 13 1 12 10
+M  V30 14 2 15 13
+M  V30 15 2 16 14
+M  V30 16 1 13 17
+M  V30 17 1 14 15
+M  V30 18 2 17 18
+M  V30 19 1 18 16
+M  V30 20 1 16 19
+M  V30 21 2 21 19
+M  V30 22 2 22 20
+M  V30 23 1 19 23
+M  V30 24 1 20 21
+M  V30 25 2 23 24
+M  V30 26 1 24 22
+M  V30 27 10 11 25
+M  V30 28 10 25 21
+M  V30 29 10 25 14
+M  V30 30 10 25 4
+M  V30 31 10 25 26
+M  V30 32 10 25 27
+M  V30 33 3 27 28
+M  V30 34 1 29 30
+M  V30 35 1 30 31
+M  V30 36 1 30 32
+M  V30 37 1 30 33
+M  V30 38 1 30 34
+M  V30 39 1 30 35
 M  V30 END BOND
 M  V30 END CTAB
@@ Line 473: / 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 483: / 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]

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Catalysts[edit | edit source]

Photosensitizer[edit | edit source]

Investigations[edit | edit source]

Sacrificial electron donor[edit | edit source]

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