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

Revision as of 10:23, 26 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 [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

100730 [Show R-Groups]

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 240: / Line 240: @@
 ====Photosensitizer ====
-<chemform smiles="C1C=C2P(C3C=CC=CC=3)(C3C=CC=CC=3)~[Re+]3(N4=C(C5N3=CC([*])=C([*])C=5)C=C([*])C([*])=C4)([C-]#[O+])([C-]#[O+])~P(C3C=CC=CC=3)(C3C=CC=CC=3)C3C=CC(P(C4C=CC=CC=4)(C4C=CC=CC=4)~[Re+]4(N5=C(C6N4=CC([*])=C([*])C=6)C=C([*])C([*])=C5)([C-]#[O+])([C-]#[O+])~P(C4C=CC=CC=4)(C4C=CC=CC=4)C4C=CC(P(C5C=CC=CC=5)(C5C=CC=CC=5)~[Re+]5(N6=CC([*])=C([*])C=C6C6C=C([*])C([*])=CN=65)([C-]#[O+])([C-]#[O+])~P(C5C=CC=CC=5)(C5C=CC=CC=5)C=1C=C2)=CC=4)=CC=3" inchi="" inchikey="" height="200px" width="300px" float="none" r1="H,CH3,CH3,H" r2="CH3,H,CH3,OMe">
+<chemform smiles="C1C=C2P(C3C=CC=CC=3)(C3C=CC=CC=3)~[Re+]3(N4=C(C5N3=CC([*])=C([*])C=5)C=C([*])C([*])=C4)([C-]#[O+])([C-]#[O+])~P(C3C=CC=CC=3)(C3C=CC=CC=3)C3C=CC(P(C4C=CC=CC=4)(C4C=CC=CC=4)~[Re+]4(N5=C(C6N4=CC([*])=C([*])C=6)C=C([*])C([*])=C5)([C-]#[O+])([C-]#[O+])~P(C4C=CC=CC=4)(C4C=CC=CC=4)C4C=CC(P(C5C=CC=CC=5)(C5C=CC=CC=5)~[Re+]5(N6=CC([*])=C([*])C=C6C6C=C([*])C([*])=CN=65)([C-]#[O+])([C-]#[O+])~P(C5C=CC=CC=5)(C5C=CC=CC=5)C=1C=C2)=CC=4)=CC=3.[P-](F)(F)(F)(F)(F)F.[P-](F)(F)(F)(F)(F)F.[P-](F)(F)(F)(F)(F)F" inchikey="" inchi="" float="none" width="200" height="200" r1="H,CH3,CH3,H" r2="CH3,H,CH3,OMe">
-   -INDIGO-02192415292D
+   -INDIGO-02262410222D
   0  0  0  0  0  0  0  0  0  0 V3000
 M  V30 BEGIN CTAB
-M  V30 COUNTS 159 183 0 0 0
+M  V30 COUNTS 180 201 0 0 0
 M  V30 BEGIN ATOM
 M  V30 1 C 6.35983 -3.83559 0.0 0
@@ Line 406: / Line 406: @@
 M  V30 158 R# 6.3044 0.786395 0.0 0 RGROUPS=(1 2)
 M  V30 159 R# 12.5314 0.789322 0.0 0 RGROUPS=(1 2)
+M  V30 160 P 16.625 -2.225 0.0 0 CHG=-1
+M  V30 161 F 16.125 -1.35897 0.0 0
+M  V30 162 F 16.125 -3.09103 0.0 0
+M  V30 163 F 17.625 -2.225 0.0 0
+M  V30 164 F 17.125 -1.35897 0.0 0
+M  V30 165 F 17.125 -3.09103 0.0 0
+M  V30 166 F 15.625 -2.225 0.0 0
+M  V30 167 P 2.775 -2.375 0.0 0 CHG=-1
+M  V30 168 F 2.275 -1.50897 0.0 0
+M  V30 169 F 2.275 -3.24103 0.0 0
+M  V30 170 F 3.775 -2.375 0.0 0
+M  V30 171 F 3.275 -1.50897 0.0 0
+M  V30 172 F 3.275 -3.24103 0.0 0
+M  V30 173 F 1.775 -2.375 0.0 0
+M  V30 174 P 9.55 -13.35 0.0 0 CHG=-1
+M  V30 175 F 9.05 -12.484 0.0 0
+M  V30 176 F 9.05 -14.216 0.0 0
+M  V30 177 F 10.55 -13.35 0.0 0
+M  V30 178 F 10.05 -12.484 0.0 0
+M  V30 179 F 10.05 -14.216 0.0 0
+M  V30 180 F 8.55 -13.35 0.0 0
 M  V30 END ATOM
 M  V30 BEGIN BOND
@@ Line 591: / Line 612: @@
 M  V30 182 1 128 158
 M  V30 183 1 135 159
+M  V30 184 1 160 161
+M  V30 185 1 160 162
+M  V30 186 1 160 163
+M  V30 187 1 160 164
+M  V30 188 1 160 165
+M  V30 189 1 160 166
+M  V30 190 1 167 168
+M  V30 191 1 167 169
+M  V30 192 1 167 170
+M  V30 193 1 167 171
+M  V30 194 1 167 172
+M  V30 195 1 167 173
+M  V30 196 1 174 175
+M  V30 197 1 174 176
+M  V30 198 1 174 177
+M  V30 199 1 174 178
+M  V30 200 1 174 179
+M  V30 201 1 174 180
 M  V30 END BOND
 M  V30 END CTAB

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

Revision as of 10:23, 26 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 10:23, 26 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