Journal Article

PUBDB-2024-06368

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Spatially and Chemically Resolved Visualization of Fe Incorporation into NiO Octahedra during the Oxygen Evolution Reaction

Yang, F. ; Lopez Luna, M. ; Haase, F. T.Extern* ; Escalera-López, D. ; Yoon, A.Extern* ; Rüscher, M.Extern* ; Rettenmaier, C.Extern* ; Jeon, H. S.Extern* ; Ortega, E. ; Timoshenko, J.Extern* ; Bergmann, A.Extern* ; Chee, S. W. (Corresponding author) ; Roldan Cuenya, B. (Corresponding author)Extern*

2023
ACS Publications Washington, DC

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Please use a persistent id in citations: doi:10.1021/jacs.3c07158  doi:10.3204/PUBDB-2024-06368

Abstract: The activity of Ni (hydr)oxides for the electrochemical evolution of oxygen (OER), a key component of the overall water splitting reaction, is known to be greatly enhanced by the incorporation of Fe. However, a complete understanding of the role of cationic Fe species and the nature of the catalyst surface under reaction conditions remains unclear. Here, using a combination of electrochemical cell and conventional transmission electron microscopy, we show how the surface of NiO electrocatalysts, with initially well-defined surface facets, restructures under applied potential and forms an active NiFe layered double (oxy)hydroxide (NiFe-LDH) when Fe3+ ions are present in the electrolyte. Continued OER under these conditions, however, leads to the creation of additional FeOx aggregates. Electrochemically, the NiFe-LDH formation correlates with a lower onset potential toward the OER, whereas the formation of the FeOx aggregates is accompanied by a gradual decrease in the OER activity. Complementary insight into the catalyst near-surface composition, structure, and chemical state is further extracted using X-ray photoelectron spectroscopy, operando Raman spectroscopy, and operando X-ray absorption spectroscopy together with measurements of Fe uptake by the electrocatalysts using time-resolved inductively coupled plasma mass spectrometry. Notably, we identified that the catalytic deactivation under stationary conditions is linked to the degradation of in situ-created NiFe-LDH. These insights exemplify the complexity of the active state formation and show how its structural and morphological evolution under different applied potentials can be directly linked to the catalyst activation and degradation.

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Contributing Institute(s):

1. DOOR-User (DOOR ; HAS-User)

Research Program(s):

1. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
2. DFG project G:(GEPRIS)388390466 - TRR 247: Heterogene Oxidationskatalyse in der Flüssigphase – Materialien und Mechanismen in der thermischen, Elektro- und Photokatalyse (388390466) (388390466)
3. OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects (725915) (725915)

Experiment(s):

1. PETRA Beamline P64 (PETRA III)

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