Imbroglio at a photoredox-iron-porphyrin catalyst dyad for the photocatalytic CO$_{{2}}$ reduction
We have covalently connected the ruthenium trisbipyridine complex (bpyRu) as a photoredox module to an iron porphyrin catalyst (porFe) through an amido function for investigating the synergistic action to power the photocatalytic CO2 reduction. The electrochemical studies of the porFe-bpyRu dyad did...
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| Format: | Article |
| Language: | English |
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Académie des sciences
2021-08-01
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| Series: | Comptes Rendus. Chimie |
| Subjects: | |
| Online Access: | https://comptes-rendus.academie-sciences.fr/chimie/articles/10.5802/crchim.104/ |
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| author | Trapali, Adelais Gotico, Philipp Herrero, Christian Ha-Thi, Minh-Huong Pino, Thomas Leibl, Winfried Charalambidis, Georgios Coutsolelos, Athanassios Halime, Zakaria Aukauloo, Ally |
| author_facet | Trapali, Adelais Gotico, Philipp Herrero, Christian Ha-Thi, Minh-Huong Pino, Thomas Leibl, Winfried Charalambidis, Georgios Coutsolelos, Athanassios Halime, Zakaria Aukauloo, Ally |
| author_sort | Trapali, Adelais |
| collection | DOAJ |
| description | We have covalently connected the ruthenium trisbipyridine complex (bpyRu) as a photoredox module to an iron porphyrin catalyst (porFe) through an amido function for investigating the synergistic action to power the photocatalytic CO2 reduction. The electrochemical studies of the porFe-bpyRu dyad did not show any marked effect on the redox properties of the constitutive units. However, the photophysical properties of the porFe-bpyRu dyad point to the complete extinction of the photoredox module that undergoes ultrafast quenching processes with the porFe acolyte, the unavoidable dilemma in this type of molecular assemblies. Nevertheless, when exogenous bpyRu and a sacrificial electron donor were added to this dyad, we found that it exhibits much higher turnover number and selectivity towards CO2 photocatalytic reduction to CO than with the iron porphyrin analogue (porFe). Comprehensive analyses of the data suggest that this catalytic enhancement displayed by the dyad can be attributed to an interesting electron relay role played by the appended bpyRu moiety. |
| first_indexed | 2024-03-11T16:13:56Z |
| format | Article |
| id | doaj.art-1a7089d286244abaa1f8d4e067cf0fd7 |
| institution | Directory Open Access Journal |
| issn | 1878-1543 |
| language | English |
| last_indexed | 2024-03-11T16:13:56Z |
| publishDate | 2021-08-01 |
| publisher | Académie des sciences |
| record_format | Article |
| series | Comptes Rendus. Chimie |
| spelling | doaj.art-1a7089d286244abaa1f8d4e067cf0fd72023-10-24T14:23:03ZengAcadémie des sciencesComptes Rendus. Chimie1878-15432021-08-0124S310111410.5802/crchim.10410.5802/crchim.104Imbroglio at a photoredox-iron-porphyrin catalyst dyad for the photocatalytic CO$_{{2}}$ reductionTrapali, Adelais0https://orcid.org/0000-0002-4495-4469Gotico, Philipp1https://orcid.org/0000-0003-2926-6016Herrero, Christian2https://orcid.org/0000-0003-2113-4625Ha-Thi, Minh-Huong3https://orcid.org/0000-0003-3276-1843Pino, Thomas4https://orcid.org/0000-0002-1646-7866Leibl, Winfried5https://orcid.org/0000-0002-2313-6643Charalambidis, Georgios6https://orcid.org/0000-0003-1237-9962Coutsolelos, Athanassios7https://orcid.org/0000-0001-5682-2968Halime, Zakaria8https://orcid.org/0000-0003-3080-9727Aukauloo, Ally9https://orcid.org/0000-0002-5480-1642Laboratory of Bioinorganic Chemistry, Chemistry Department, University of Crete, PO Box 2208, 71003 Heraklion, Crete, GreeceUniversité Paris-Saclay, CNRS, Institut des Sciences Moléculaires d’Orsay (ISMO), 91405, Orsay, FranceUniversité Paris-Saclay, CNRS, Institut de Chimie Moléculaire et des Matériaux d’Orsay (ICMMO), 91405, Orsay, FranceUniversité Paris-Saclay, CNRS, Institut des Sciences Moléculaires d’Orsay (ISMO), 91405, Orsay, FranceUniversité Paris-Saclay, CNRS, Institut des Sciences Moléculaires d’Orsay (ISMO), 91405, Orsay, FranceUniversité Paris-Saclay, CEA, Institute for Integrative Biology of the Cell (I2BC), 91198, Gif-sur-Yvette, FranceLaboratory of Bioinorganic Chemistry, Chemistry Department, University of Crete, PO Box 2208, 71003 Heraklion, Crete, GreeceLaboratory of Bioinorganic Chemistry, Chemistry Department, University of Crete, PO Box 2208, 71003 Heraklion, Crete, GreeceUniversité Paris-Saclay, CNRS, Institut de Chimie Moléculaire et des Matériaux d’Orsay (ICMMO), 91405, Orsay, FranceUniversité Paris-Saclay, CNRS, Institut de Chimie Moléculaire et des Matériaux d’Orsay (ICMMO), 91405, Orsay, France; Université Paris-Saclay, CEA, Institute for Integrative Biology of the Cell (I2BC), 91198, Gif-sur-Yvette, FranceWe have covalently connected the ruthenium trisbipyridine complex (bpyRu) as a photoredox module to an iron porphyrin catalyst (porFe) through an amido function for investigating the synergistic action to power the photocatalytic CO2 reduction. The electrochemical studies of the porFe-bpyRu dyad did not show any marked effect on the redox properties of the constitutive units. However, the photophysical properties of the porFe-bpyRu dyad point to the complete extinction of the photoredox module that undergoes ultrafast quenching processes with the porFe acolyte, the unavoidable dilemma in this type of molecular assemblies. Nevertheless, when exogenous bpyRu and a sacrificial electron donor were added to this dyad, we found that it exhibits much higher turnover number and selectivity towards CO2 photocatalytic reduction to CO than with the iron porphyrin analogue (porFe). Comprehensive analyses of the data suggest that this catalytic enhancement displayed by the dyad can be attributed to an interesting electron relay role played by the appended bpyRu moiety.https://comptes-rendus.academie-sciences.fr/chimie/articles/10.5802/crchim.104/Supramolecular dyadIron porphyrinsCarbon dioxide reductionPhotocatalysisFlash photolysis |
| spellingShingle | Trapali, Adelais Gotico, Philipp Herrero, Christian Ha-Thi, Minh-Huong Pino, Thomas Leibl, Winfried Charalambidis, Georgios Coutsolelos, Athanassios Halime, Zakaria Aukauloo, Ally Imbroglio at a photoredox-iron-porphyrin catalyst dyad for the photocatalytic CO$_{{2}}$ reduction Comptes Rendus. Chimie Supramolecular dyad Iron porphyrins Carbon dioxide reduction Photocatalysis Flash photolysis |
| title | Imbroglio at a photoredox-iron-porphyrin catalyst dyad for the photocatalytic CO$_{{2}}$ reduction |
| title_full | Imbroglio at a photoredox-iron-porphyrin catalyst dyad for the photocatalytic CO$_{{2}}$ reduction |
| title_fullStr | Imbroglio at a photoredox-iron-porphyrin catalyst dyad for the photocatalytic CO$_{{2}}$ reduction |
| title_full_unstemmed | Imbroglio at a photoredox-iron-porphyrin catalyst dyad for the photocatalytic CO$_{{2}}$ reduction |
| title_short | Imbroglio at a photoredox-iron-porphyrin catalyst dyad for the photocatalytic CO$_{{2}}$ reduction |
| title_sort | imbroglio at a photoredox iron porphyrin catalyst dyad for the photocatalytic co 2 reduction |
| topic | Supramolecular dyad Iron porphyrins Carbon dioxide reduction Photocatalysis Flash photolysis |
| url | https://comptes-rendus.academie-sciences.fr/chimie/articles/10.5802/crchim.104/ |
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