Journal Article

PUBDB-2024-05256

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Applying Nuclear Forward Scattering as In Situ and Operando Tool for the Characterization of $FeN_4$ Moieties in the Hydrogen Evolution Reaction

Heppe, N.Extern* ; Gallenkamp, C. ; Snitkoff-Sol, R. Z. ; Paul, S. D.Extern* ; Segura-Salas, N. ; Haak, H.Extern* ; Moritz, D. C. ; Kaiser, B. ; Jaegermann, W. ; Potapkin, V.Extern* ; Jafari, A.Extern*DESY* ; Schünemann, V.Extern* ; Leupold, O.XFEL.EU*DESY* ; Elbaz, L. ; Krewald, V. ; Kramm, U. (Corresponding author)Extern*

2024
ACS Publications Washington, DC

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Please use a persistent id in citations: doi:10.1021/jacs.4c00436  doi:10.3204/PUBDB-2024-05256

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.

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Contributing Institute(s):

1. DOOR-User (DOOR ; HAS-User)
2. Experimentebetreuung PETRA III (FS-PET-S)

Research Program(s):

1. 632 - Materials – Quantum, Complex and Functional Materials (POF4-632) (POF4-632)
2. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
3. FS-Proposal: I-20200863 (I-20200863) (I-20200863)
4. FS-Proposal: I-20221267 (I-20221267) (I-20221267)
5. DFG project 443703006 - SFB 1487: Eisen, neu gedacht! (443703006) (443703006)

Experiment(s):

1. PETRA Beamline P01 (PETRA III)

Appears in the scientific report 2024

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Database coverage:
; ; ; BIOSIS Previews ; Biological Abstracts ; Chemical Reactions ; Clarivate Analytics Master Journal List ; Current Contents - Life Sciences ; Current Contents - Physical, Chemical and Earth Sciences ; Ebsco Academic Search ; Essential Science Indicators ; IF >= 15 ; Index Chemicus ; JCR ; Nationallizenz ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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