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

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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 [Mn(dtBubpy)(CO)3(MeCN)][PF6] 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 [Mn(dtBubpy)(CO)3(MeCN)][PF6]

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

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+M  V30 132 C 9.86335 0.787792 0.0 0
-M  V30 133 C 10.7617 2.60386 0.0 0
+M  V30 133 C 11.1959 1.55881 0.0 0
-M  V30 134 C 9.76407 2.60412 0.0 0
+M  V30 134 C 10.3082 1.55904 0.0 0
-M  V30 135 C 11.2628 1.73735 0.0 0
+M  V30 135 C 11.6417 0.787854 0.0 0
-M  V30 136 N 9.7671 0.867312 0.0 0
+M  V30 136 N 10.3109 0.0137595 0.0 0
-M  V30 137 C 10.7672 0.873775 0.0 0
+M  V30 137 C 11.2008 0.0195098 0.0 0
-M  V30 138 R# 11.2617 3.46988 0.0 0 RGROUPS=(1 1)
+M  V30 138 R# 11.6407 2.32933 0.0 0 RGROUPS=(1 1)
-M  V30 139 R# 6.2636 3.46464 0.0 0 RGROUPS=(1 1)
+M  V30 139 R# 7.19379 2.32467 0.0 0 RGROUPS=(1 1)
-M  V30 140 C 3.60504 -11.4417 0.0 0
+M  V30 140 C 4.8284 -10.9379 0.0 0
-M  V30 141 C 2.1068 -12.3073 0.0 0
+M  V30 141 C 3.49538 -11.708 0.0 0
-M  V30 142 C 3.10443 -12.3082 0.0 0
+M  V30 142 C 4.38299 -11.7088 0.0 0
-M  V30 143 C 1.60632 -11.4404 0.0 0
+M  V30 143 C 3.05009 -10.9367 0.0 0
-M  V30 144 N 3.10257 -10.5714 0.0 0
+M  V30 144 N 4.38134 -10.1636 0.0 0
-M  V30 145 C 2.10251 -10.5772 0.0 0
+M  V30 145 C 3.49156 -10.1687 0.0 0
-M  V30 146 C 1.60251 -9.71116 0.0 0
+M  V30 146 C 3.0467 -9.39818 0.0 0
-M  V30 147 C 0.1032 -8.84744 0.0 0
+M  V30 147 C 1.71272 -8.6297 0.0 0
-M  V30 148 C 0.601793 -9.71154 0.0 0
+M  V30 148 C 2.15633 -9.39851 0.0 0
-M  V30 149 C 0.60309 -7.98026 0.0 0
+M  V30 149 C 2.15749 -7.85815 0.0 0
-M  V30 150 N 2.1044 -8.84052 0.0 0
+M  V30 150 N 3.49324 -8.62354 0.0 0
-M  V30 151 C 1.59877 -7.97768 0.0 0
+M  V30 151 C 3.04337 -7.85585 0.0 0
-M  V30 152 R# -0.8968 -8.84744 0.0 0 RGROUPS=(1 1)
+M  V30 152 R# 0.822997 -8.6297 0.0 0 RGROUPS=(1 1)
-M  V30 153 R# 1.6068 -13.1733 0.0 0 RGROUPS=(1 1)
+M  V30 153 R# 3.05051 -12.4785 0.0 0 RGROUPS=(1 1)
-M  V30 154 R# 3.60443 -13.1742 0.0 0 RGROUPS=(1 2)
+M  V30 154 R# 4.82786 -12.4793 0.0 0 RGROUPS=(1 2)
-M  V30 155 R# 0.101678 -7.11505 0.0 0 RGROUPS=(1 2)
+M  V30 155 R# 1.71137 -7.08835 0.0 0 RGROUPS=(1 2)
-M  V30 156 R# 14.114 -13.1579 0.0 0 RGROUPS=(1 2)
+M  V30 156 R# 14.1785 -12.4648 0.0 0 RGROUPS=(1 2)
-M  V30 157 R# 17.6106 -7.0952 0.0 0 RGROUPS=(1 2)
+M  V30 157 R# 17.2895 -7.07069 0.0 0 RGROUPS=(1 2)
-M  V30 158 R# 5.26398 1.73571 0.0 0 RGROUPS=(1 2)
+M  V30 158 R# 6.3044 0.786395 0.0 0 RGROUPS=(1 2)
-M  V30 159 R# 12.2628 1.739 0.0 0 RGROUPS=(1 2)
+M  V30 159 R# 12.5314 0.789322 0.0 0 RGROUPS=(1 2)
 M  V30 END ATOM
 M  V30 BEGIN BOND

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

Revision as of 15:29, 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 15:29, 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