Applying Nuclear Forward Scattering as In Situ and Operando Tool for the Characterization of FeN4 Moieties in the Hydrogen Evolution Reaction

Nils Heppe, Charlotte Gallenkamp, Rifael Z. Snitkoff-Sol, Stephen D. Paul, Nicole Segura-Salas, Hendrik Haak, Dominik C. Moritz, Bernhard Kaiser, Wolfram Jaegermann, Vasily Potapkin, Atefeh Jafari, Volker Schünemann, Olaf Leupold, Lior Elbaz, Vera Krewald, Ulrike I. Kramm

Research output: Contribution to journalArticlepeer-review

Abstract

Nuclear forward scattering (NFS) is a synchrotron-based technique relying on the recoil-free nuclear resonance effect similar to Mössbauer spectroscopy. In this work, we introduce NFS for in situ and operando measurements during electrocatalytic reactions. The technique enables faster data acquisition and better discrimination of certain iron sites in comparison to Mössbauer spectroscopy. It is directly accessible at various synchrotrons to a broad community of researchers and is applicable to multiple metal isotopes. We demonstrate the power of this technique with the hydrogen evolution mechanism of an immobilized iron porphyrin supported on carbon. Such catalysts are often considered as model systems for iron-nitrogen-carbon (FeNC) catalysts. Using in situ and operando NFS in combination with theoretical predictions of spectroscopic data enables the identification of the intermediate that is formed prior to the rate-determining step. The conclusions on the reaction mechanism can be used for future optimization of immobilized molecular catalysts and metal-nitrogen-carbon (MNC) catalysts.

Original languageEnglish
JournalJournal of the American Chemical Society
Early online date17 Apr 2024
DOIs
StatePublished - 8 May 2024

Bibliographical note

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© 2024 The Authors. Published by American Chemical Society.

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