TUdatalib : Substituent Effects in Iron Porphyrin Catalysts for the Hydrogen Evolution Reaction

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dc.contributor.author	Heppe, Nils
dc.contributor.author	Gallenkamp, Charlotte
dc.contributor.author	Paul, Stephen
dc.contributor.author	Segura-Salas, Nicole
dc.contributor.author	von Rhein, Niklas
dc.contributor.author	Kaiser, Bernhard
dc.contributor.author	Jaegermann, Wolfram
dc.contributor.author	Jafari, Atefeh
dc.contributor.author	Sergueev, Ilya
dc.contributor.author	Krewald, Vera
dc.contributor.author	Kramm, Ulrike Ingrid
dc.date.accessioned	2022-12-09T17:44:53Z
dc.date.available	2022-12-09T17:44:53Z
dc.date.issued	2022
dc.identifier.uri	https://tudatalib.ulb.tu-darmstadt.de/handle/tudatalib/3674
dc.description	Data package used for the peer-reviewed publication: "Substituent Effects in Iron Porphyrin Catalysts for the Hydrogen Evolution Reaction" in Chemistry - A European Journal. DOI: 10.1002/chem.202202465 Abstract: For a future hydrogen economy, non-precious metal catalysts for the water splitting reactions are needed that can be implemented on a global scale. Metal-nitrogen-carbon (MNC) catalysts with active sites constituting a metal center with fourfold coordination of nitrogen (MN4) show promising performance, but an optimization rooted in structure-property relationships has been hampered by their low structural definition. Porphyrin model complexes are studied to transfer insights from well-defined molecules to MNC systems. This work combines experiment and theory to evaluate the influence of porphin substituents on the electronic and electrocatalytic properties of MN4 centers with respect to the hydrogen evolution reaction (HER) in aqueous electrolyte. We found that the choice of substituent affects their utilization on the carbon support and their electrocatalytic performance. We propose an HER mechanism for supported iron porphyrin complexes involving a [FeII(P▪)]- radical anion intermediate, in which a porphinic nitrogen atom acts as an internal base. While this work focuses on the HER, the limited influence of a simultaneous interaction with the support and an aqueous electrolyte will likely be transferrable to other catalytic applications.	de_DE
dc.language.iso	en	de_DE
dc.relation	IsSupplementTo;DOI;10.1002/chem.202202465
dc.rights	Open Data Commons Attribution License (ODC-By) v1.0
dc.rights.uri	https://opendatacommons.org/licenses/by/1.0/
dc.subject	Density functional theory;Electrochemistry;Heterogeneous catalysis;Hydrogen;Molecular electrochemistry;Renewable resources	de_DE
dc.subject.classification	3.12-02 Physikalische Chemie von Festkörpern und Oberflächen, Materialcharakterisierung	de_DE
dc.subject.ddc	540
dc.title	Substituent Effects in Iron Porphyrin Catalysts for the Hydrogen Evolution Reaction	de_DE
dc.type	Dataset	de_DE
dc.description.version	DOI:10.1002/chem.202202465	de_DE
tud.unit	TUDa
tud.history.classification	Version=2020-2024;322-02 Physikalische Chemie von Festkörpern und Oberflächen, Materialcharakterisierung