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Remote ion-pair interactions in Fe-porphyrin-based molecular catalysts for the hydrogen evolution reaction

Abstract

The environmentally benign production of clean energies is extremely important for the sustainable progress of our society. In this respect, dihydrogen (H2) has been considered in the last decades as an efficient energy carrier and much effort has been directed to the hydrogen evolution reaction (HER. Herein, we report on the efficiency of iron-based 5,10,15,20-tetraphenylporphyrins containing carboxylate groups at different positions (ortho, meta and para of the meso-substituted aryl groups of the porphyrin backbone) as molecular catalysts for the HER. We found that, besides stereoelectronic control, the subttle differences observed in the cyclic voltammograms (CV) as well as those associated to the electrocatalytic activity might involve a previously neglected, ion-pair interaction between the carboxylate groups of the porphyrin scaffold and the chloride anions belonging to the commonly used proton source Et3NHCl. In particular, the iron-based porphyrin containing the carboxylic acids in ortho position was found completely inactive in HER, which highlights the relevance of ion-pair contacts remote from the active center for this type of catalytic systems.

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Publication details

The article was received on 18 Oct 2018, accepted on 07 Feb 2019 and first published on 08 Feb 2019


Article type: Paper
DOI: 10.1039/C8CY02164C
Citation: Catal. Sci. Technol., 2019, Accepted Manuscript

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    Remote ion-pair interactions in Fe-porphyrin-based molecular catalysts for the hydrogen evolution reaction

    S. Kasemthaveechok, B. Fabre, G. Loget and R. Gramage-Doria, Catal. Sci. Technol., 2019, Accepted Manuscript , DOI: 10.1039/C8CY02164C

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