Journal Article PUBDB-2023-07339

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Systematic in situ Investigation of the Formation of NH$_3$ Cracking Catalysts from Precursor Perovskites ABO$_3$ (A=La,Ca,Sr and B=Fe,Co,Ni) and their Catalytic Performance

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2023
Wiley-VCH Weinheim

ChemCatChem 15(21), e202300947 () [10.1002/cctc.202300947]
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Abstract: This work addresses the formation of ammonia (NH$_3$) decomposition catalysts derived from perovskites ABO$_3$ (A=La, Ca, Sr, and B=Fe, Co, Ni) precursors via operando synchrotron X-ray diffraction experiments. During the reaction in NH$_3$, the perovskite precursors are decomposed and the transition metals are reduced. Depending on their reduction properties, active metallic catalysts are formed in situ on La$_2$O$_3$ as support. The reduction behavior of the perovskites, formation of intermediate phases during activation, and catalytic performance was studied in detail. In addition, microstructure properties such as crystallite sizes and particle morphology were analyzed. Co-/Ni-based perovskites decomposed completely during activation to Co$_0$/Ni$_0$ supported on La$_2$O$_3$ while Fe-based perovskites were fully stable but inactive in catalysis. This difference is due to varying electronic properties of the transition metals, e. g., decreasing electronegativity from Ni to Fe. With decreasing reducibility, the intermediate phases during activation formed more distinct. La$^{3+}$ was partially substituted by Ca$^{2+}$/Sr$^{2+}$ in LaCoO$_3$ to test for advantageous effects in NH$_3$ decomposition. The best performance was observed using the precatalyst La$_{0.8}$Sr$_{0.2}$CoO$_3$ with a conversion of 86 % (100 % NH$_3$, 15000 mL g$^{−1}$ h$^{−1}$) at 550 °C.

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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)
Experiment(s):
  1. PETRA Beamline P02.1 (PETRA III)

Appears in the scientific report 2023
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Medline ; Clarivate Analytics Master Journal List ; Current Contents - Physical, Chemical and Earth Sciences ; Ebsco Academic Search ; IF < 5 ; JCR ; SCOPUS ; Web of Science Core Collection
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 Record created 2023-11-29, last modified 2025-07-24


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