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@ARTICLE{Heppe:612269,
author = {Heppe, Nils and Gallenkamp, Charlotte and Snitkoff-Sol,
Rifael Z. and Paul, Stephen D. and Segura-Salas, Nicole and
Haak, Hendrik and Moritz, Dominik C. and Kaiser, Bernhard
and Jaegermann, Wolfram and Potapkin, Vasily and Jafari,
Atefeh and Schünemann, Volker and Leupold, Olaf and Elbaz,
Lior and Krewald, Vera and Kramm, Ulrike},
title = {{A}pplying {N}uclear {F}orward {S}cattering as {I}n {S}itu
and {O}perando {T}ool for the {C}haracterization of
${F}e{N}_4$ {M}oieties in the {H}ydrogen {E}volution
{R}eaction},
journal = {Journal of the American Chemical Society},
volume = {146},
number = {18},
issn = {0002-7863},
address = {Washington, DC},
publisher = {ACS Publications},
reportid = {PUBDB-2024-05256},
pages = {12496-12510},
year = {2024},
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.},
cin = {DOOR ; HAS-User / FS-PET-S},
ddc = {540},
cid = {I:(DE-H253)HAS-User-20120731 /
I:(DE-H253)FS-PET-S-20190712},
pnm = {632 - Materials – Quantum, Complex and Functional
Materials (POF4-632) / 6G3 - PETRA III (DESY) (POF4-6G3) /
FS-Proposal: I-20200863 (I-20200863) / FS-Proposal:
I-20221267 (I-20221267) / DFG project 443703006 - SFB 1487:
Eisen, neu gedacht! (443703006)},
pid = {G:(DE-HGF)POF4-632 / G:(DE-HGF)POF4-6G3 /
G:(DE-H253)I-20200863 / G:(DE-H253)I-20221267 /
G:(GEPRIS)443703006},
experiment = {EXP:(DE-H253)P-P01-20150101},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:38630640},
UT = {WOS:001226283100001},
doi = {10.1021/jacs.4c00436},
url = {https://bib-pubdb1.desy.de/record/612269},
}