Ladungsunterstützte Selbstmetallierung von Porphyrinen auf Oxidoberflächen

Das Interesse an Metallierungs-und Selbstmetallierungsreaktionen auf Oxidoberflächen ist in jüngster Zeit ständig gewachsen. Der Mechanismus der Selbstmetallierungsreaktion ist jedoch nicht vollständig geklärt. Hier zeigen wir mithilfe von Rastertunnelmikroskopie, Photoemissions-Spektroskopie und Dichtefunktionaltheorie-Rechnungen, dass die Selbstmetallierung von 2H-Tetraphenylporphyrin auf der Oberfläche von ultradünnen MgO(001)-Filmen durch Ladungstransfer ermçglicht wird. Es wird gezeigt, dass der Ladungszustand und dadurch der Metallierungszustand der Porphyrin-Moleküle durch die Austrittsarbeit des MgO(001)/ Ag(001)-Substrats gezielt eingestellt werden kçnnen.

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Ladungsunterstützte Selbstmetallierung von Porphyrinen auf Oxidoberflächen

Egger

Hollerer

Kern

et al. 2021

Angewandte Chemie

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Self‐Metalation of Porphyrins at the Solid–Gas Interface

et al. 2021

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Self-metalation is ap romising route to include as ingle metal atom in at etrapyrrolic macrocycle in organic frameworks supported by metal surfaces.T he molecule-surface interaction may providet he charge transfer and the geometric distortion of the molecular plane necessary for metal inclusion. However,a tametal surface the presence of an activation barrier can represent an obstacle that cannot be compensated by ah igher substrate temperature without affecting the layer integrity.The formation of the intermediate state can be facilitated in some cases by oxygen pre-adsorption at the supporting metal surface,l ike in the case of 2H-TPP/ Pd(100). In such cases,the activation barrier can be overcome by mild annealing,y ielding the formation of desorbing products and of the metalated tetrapyrrole.W eshow here that the self-metalation of 2H-TPP at the Pd(100) surface can be promoted already at room temperature by the presence of an oxygen gas phase at close-to-ambient conditions via an Eley-Rideal mechanism.

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Self‐Metalation of Porphyrins at the Solid–Gas Interface

et al. 2021

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Ladungsunterstützte Selbstmetallierung von Porphyrinen auf Oxidoberflächen

Cited by 3 publications

References 25 publications