Rhenium(I) trinuclear rings as highly efficient redox photosensitizers for photocatalytic CO2 reduction: Difference between revisions

Revision as of 15:19, 19 February 2024

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Abstract

Summary

A photochemical reduction of CO₂ to CO or formic acid was shown using the bipyridine-based rhenium, ruthenium and manganese catalysts [Re(bpy)(CO)3(MeCN)][PF6], Ru(dtBubpy)(CO)2Cl2 or Molecule with key WCQGNVNGTWFVLO-UHFFFAOYSA-N does not exist. in combination with cyclic rhenium-based trinuclear redox photosensitizers. Turnover numbers (TONs) of up to 290 for formic acid were reached in DMA with the ruthenium complex Ru(dtBubpy)(CO)2Cl2 and photosensitizer Molecule with key KSOIVZAANOLODS-UHFFFAOYSA-T does not exist.. For CO production, TONs of up to 98 were obtained in DMF with the rhenium complex [Re(bpy)(CO)3(MeCN)][PF6] and photosensitizer Molecule with key LOLRMPNEYKEGPF-UHFFFAOYSA-T does not exist.. The experiments were conducted under visible-light irradiation (λ = 436 nm) using TEOA as sacrificial electron donor (see section SEDs below).

Advances and special progress

Re(I)-based trinuclear photosensitizers were developed and allowed for high product selectivities for CO or formic acid in CO₂ reduction attempts with different bipyridine-based catalysts.

Additional remarks

Content of the published article in detail

The article contains results for the reduction of CO₂ to CO or formic acid under visible-light catalysis using bipyridine-based complexes and rhenium-based trinuclear rings as photosensitizers. The catalytic system performs best in DMA for formic acid production (referring to the TON of formic acid production) and in DMF for CO production.

Catalyst

[Re(bpy)(CO)3(MeCN)][PF6] Ru(dtBubpy)(CO)2Cl2

Photosensitizer

Investigation

	cat	cat conc [µM]	PS	PS conc [mM]	solvent A	λexc [nm]	TON CO
1.	[Re(bpy)(CO)3(MeCN)][PF6]	0.05	Molecule:100878	0.05	DMF	436	27
2.	[Re(bpy)(CO)3(MeCN)][PF6]	0.05	Molecule:100878	0.05	DMF	436	98
3.	[Re(bpy)(CO)3(MeCN)][PF6]	0.05	Molecule:100877	0.05	DMF	436	22
4.	[Re(bpy)(CO)3(MeCN)][PF6]	0.05	Molecule:100877	0.05	DMF	436	71
5.			Molecule:100877	0.05	DMF	436	6
6.			Molecule:100877	0.05	DMF	436	8
7.	[Re(bpy)(CO)3(MeCN)][PF6]	0.05	Molecule:100879	0.05	DMF	436	20
8.	[Re(bpy)(CO)3(MeCN)][PF6]	0.05	Molecule:100879	0.05	DMF	436	32
9.	[Re(bpy)(CO)3(MeCN)][PF6]	0.05	Molecule:100880	0.05	DMF	436	11
10.	[Re(bpy)(CO)3(MeCN)][PF6]	0.05	Molecule:100880	0.05	DMF	436	48

Investigation-Name: Table 1

	cat	cat conc [µM]	PS	PS conc [mM]	e-D	e-D conc [M]	solvent A	λexc [nm]	TON CO	TON H2	TON HCOOH
1.	Ru(dtBubpy)(CO)2Cl2	0.05	Molecule:100877	0.05			DMF	436	20	72	290
2.	Ru(dtBubpy)(CO)2Cl2	0.05	Molecule:100877	0.05	BI(OH)H	0.03	DMF	436	16	49	280
3.	[Mn(dtBubpy)(CO)3(MeCN)][PF6]	0.05	Molecule:100877	0.05			DMF	436	32		85
4.	[Mn(dtBubpy)(CO)3(MeCN)][PF6]	0.05	Molecule:100877	0.05	BI(OH)H	0.03	DMF	436	80		60

Investigation-Name: Table 2

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

Table 1 (Molecular process, Photocatalytic CO2 conversion experiments)
Table 2 (Molecular process, Photocatalytic CO2 conversion experiments)

DOI	10.1039/c6sc01913g
Authors	Jana Rohacova, Osamu Ishitani,
Submitted	05.07.2016
Published online	2016
Licenses	-
Subjects	-
Go to literature page

@@ Line 150: / Line 150: @@
 M  V30 END CTAB
 M  END
-</chemform><chemform smiles="" inchi="" inchikey="OMERWMHUIAGAOR-UHFFFAOYSA-N" height="200px" width="300px" float="none"></chemform>
+</chemform><chemform smiles="C(C(C)(C)C)1C=C2C3C=C(C(C)(C)C)C=CN=3[Mn+](C#O)(C#O)(C#O)(N#CC)N2=CC=1.F[P-](F)(F)(F)(F)F" inchi="1S/C18H24N2.C2H3N.3CHO.F6P.Mn/c1-17(2,3)13-7-9-19-15(11-13)16-12-14(8-10-20-16)18(4,5)6;1-2-3;3*1-2;1-7(2,3,4,5)6;/h7-12H,1-6H3;1H3;3*1H;;/q;;;;;-1;+1" inchikey="WCQGNVNGTWFVLO-UHFFFAOYSA-N" height="200px" width="300px" float="none">
+  -INDIGO-02192415192D
+  0  0  0  0  0  0  0  0  0  0 V3000
+M  V30 BEGIN CTAB
+M  V30 COUNTS 37 38 0 0 0
+M  V30 BEGIN ATOM
+M  V30 1 C 5.54029 -0.252784 0.0 0
+M  V30 2 C 7.12769 -0.252344 0.0 0
+M  V30 3 C 6.3355 0.206014 0.0 0
+M  V30 4 N 7.12769 -1.17062 0.0 0
+M  V30 5 C 5.54029 -1.17474 0.0 0
+M  V30 6 C 6.3375 -1.62887 0.0 0
+M  V30 7 C 6.3375 -2.54628 0.0 0
+M  V30 8 C 7.13251 -3.92025 0.0 0
+M  V30 9 N 7.13275 -3.00501 0.0 0
+M  V30 10 C 6.33756 -4.37993 0.0 0
+M  V30 11 C 5.53938 -3.00779 0.0 0
+M  V30 12 C 5.5453 -3.92525 0.0 0
+M  V30 13 C 4.74579 0.205922 0.0 0
+M  V30 14 C 3.85964 -0.0315228 0.0 0
+M  V30 15 C 3.95129 0.664629 0.0 0
+M  V30 16 C 4.50834 1.09207 0.0 0
+M  V30 17 C 4.75081 -4.38396 0.0 0
+M  V30 18 C 3.9563 -4.84267 0.0 0
+M  V30 19 C 3.86465 -4.14651 0.0 0
+M  V30 20 C 4.51336 -5.27012 0.0 0
+M  V30 21 Mn 7.75598 -2.06461 0.0 0 CHG=1
+M  V30 22 N 7.75598 -1.1472 0.0 0
+M  V30 23 C 8.55048 -1.6059 0.0 0
+M  V30 24 C 8.55048 -2.52332 0.0 0
+M  V30 25 C 7.99343 -2.95077 0.0 0
+M  V30 26 C 7.75598 -0.229785 0.0 0
+M  V30 27 C 7.75598 0.687628 0.0 0
+M  V30 28 O 9.34499 -1.1472 0.0 0
+M  V30 29 O 9.34499 -2.98202 0.0 0
+M  V30 30 O 8.23087 -3.83691 0.0 0
+M  V30 31 F 11.3568 2.70594 0.0 0
+M  V30 32 P 12.5485 3.394 0.0 0 CHG=-1 VAL=6
+M  V30 33 F 12.5485 2.01788 0.0 0
+M  V30 34 F 13.7404 2.70594 0.0 0
+M  V30 35 F 12.5485 4.77012 0.0 0
+M  V30 36 F 13.7404 4.08206 0.0 0
+M  V30 37 F 11.3568 4.08206 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 6 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 1 1 13
+M  V30 15 1 13 14
+M  V30 16 1 13 15
+M  V30 17 1 13 16
+M  V30 18 1 12 17
+M  V30 19 1 17 18
+M  V30 20 1 17 19
+M  V30 21 1 17 20
+M  V30 22 10 4 21
+M  V30 23 10 9 21
+M  V30 24 10 21 22
+M  V30 25 10 21 23
+M  V30 26 10 21 24
+M  V30 27 10 21 25
+M  V30 28 3 22 26
+M  V30 29 1 26 27
+M  V30 30 3 23 28
+M  V30 31 3 24 29
+M  V30 32 3 25 30
+M  V30 33 1 31 32
+M  V30 34 1 32 33
+M  V30 35 1 32 34
+M  V30 36 1 32 35
+M  V30 37 1 32 36
+M  V30 38 1 32 37
+M  V30 END BOND
+M  V30 END CTAB
+M  END
+</chemform>
 ====Photosensitizer ====

Rhenium(I) trinuclear rings as highly efficient redox photosensitizers for photocatalytic CO2 reduction: Difference between revisions

Revision as of 15:19, 19 February 2024

Contents

Abstract

Summary

Advances and special progress

Additional remarks

Content of the published article in detail

Catalyst

Photosensitizer

Investigation

Sacrificial Electron Donor

Additives

Investigations

Topics

Rhenium(I) trinuclear rings as highly efficient redox photosensitizers for photocatalytic CO2 reduction: Difference between revisions

Revision as of 15:19, 19 February 2024

Abstract

Summary

Advances and special progress

Additional remarks

Content of the published article in detail

Catalyst

Photosensitizer

Investigation

Sacrificial Electron Donor

Additives

Investigations

Current site

Topics