Papadakis, Michael ; Barrozo, Alexandre ; Delmotte, Léa ; Straistari, Tatiana ; Shova, Sergiu ; Réglier, Marius ; Krewald, Vera ; Bertaina, Sylvain ; Hardré, Renaud ; Orio, Maylis (2023)
How Metal Nuclearity Impacts Electrocatalytic H₂ Production in Thiocarbohydrazone-Based Complexes.
In: Inorganics, 2023, 11 (4)
doi: 10.26083/tuprints-00023650
Artikel, Zweitveröffentlichung, Verlagsversion
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Kurzbeschreibung (Abstract)
Thiocarbohydrazone-based catalysts feature ligands that are potentially electrochemically active. From the synthesis point of view, these ligands can be easily tailored, opening multiple strategies for optimization, such as using different substituent groups or metal substitution. In this work, we show the possibility of a new strategy, involving the nuclearity of the system, meaning the number of metal centers. We report the synthesis and characterization of a trinuclear nickel-thiocarbohydrazone complex displaying an improved turnover rate compared with its mononuclear counterpart. We use DFT calculations to show that the mechanism involved is metal-centered, unlike the metal-assisted ligand-centered mechanism found in the mononuclear complex. Finally, we show that two possible mechanisms can be assigned to this catalyst, both involving an initial double reduction of the system.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2023 |
| Autor(en): | Papadakis, Michael ; Barrozo, Alexandre ; Delmotte, Léa ; Straistari, Tatiana ; Shova, Sergiu ; Réglier, Marius ; Krewald, Vera ; Bertaina, Sylvain ; Hardré, Renaud ; Orio, Maylis |
| Art des Eintrags: | Zweitveröffentlichung |
| Titel: | How Metal Nuclearity Impacts Electrocatalytic H₂ Production in Thiocarbohydrazone-Based Complexes |
| Sprache: | Englisch |
| Publikationsjahr: | 2023 |
| Ort: | Darmstadt |
| Publikationsdatum der Erstveröffentlichung: | 2023 |
| Verlag: | MDPI |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Inorganics |
| Jahrgang/Volume einer Zeitschrift: | 11 |
| (Heft-)Nummer: | 4 |
| Kollation: | 19 Seiten |
| DOI: | 10.26083/tuprints-00023650 |
| URL / URN: | https://tuprints.ulb.tu-darmstadt.de/23650 |
| Zugehörige Links: | |
| Herkunft: | Zweitveröffentlichung DeepGreen |
| Kurzbeschreibung (Abstract): | Thiocarbohydrazone-based catalysts feature ligands that are potentially electrochemically active. From the synthesis point of view, these ligands can be easily tailored, opening multiple strategies for optimization, such as using different substituent groups or metal substitution. In this work, we show the possibility of a new strategy, involving the nuclearity of the system, meaning the number of metal centers. We report the synthesis and characterization of a trinuclear nickel-thiocarbohydrazone complex displaying an improved turnover rate compared with its mononuclear counterpart. We use DFT calculations to show that the mechanism involved is metal-centered, unlike the metal-assisted ligand-centered mechanism found in the mononuclear complex. Finally, we show that two possible mechanisms can be assigned to this catalyst, both involving an initial double reduction of the system. |
| Freie Schlagworte: | hydrogen evolution, bio-inspiration, electrocatalysis, quantum chemistry, reaction mechanism |
| Status: | Verlagsversion |
| URN: | urn:nbn:de:tuda-tuprints-236500 |
| Zusätzliche Informationen: | This article belongs to the Special Issue Women’s Special Issue Series: Inorganics |
| Sachgruppe der Dewey Dezimalklassifikatin (DDC): | 500 Naturwissenschaften und Mathematik > 540 Chemie |
| Fachbereich(e)/-gebiet(e): | 07 Fachbereich Chemie Zentrale Einrichtungen Zentrale Einrichtungen > Hochschulrechenzentrum (HRZ) Zentrale Einrichtungen > Hochschulrechenzentrum (HRZ) > Hochleistungsrechner 07 Fachbereich Chemie > Theoretische Chemie (am 07.02.2024 umbenannt in Quantenchemie) |
| Hinterlegungsdatum: | 11 Apr 2023 11:35 |
| Letzte Änderung: | 01 Aug 2024 08:49 |
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| Suche nach Titel in: | TUfind oder in Google |
Verfügbare Versionen dieses Eintrags
- How Metal Nuclearity Impacts Electrocatalytic H₂ Production in Thiocarbohydrazone-Based Complexes. (deposited 11 Apr 2023 11:35) [Gegenwärtig angezeigt]
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