Journal Article

PUBDB-2025-03912

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Role of Gas Dropouts in CO₂ Methanation over MOF‐Derived Ni₃Fe@C Catalysts: An In Situ XAS and PDF Study

Manzoni, F.Extern* ; Strübbe, S.Extern* ; Rohrbach, L. ; Boniface, M. ; Lunkenbein, T.Extern* ; Schoch, R.Extern* ; Kleist, W.Extern* ; Bauer, M. (Corresponding author)Extern* ; Zobel, M. (Corresponding author)Extern*

2025
Wiley-VCH Weinheim

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Please use a persistent id in citations: doi:10.1002/cctc.202500859  doi:10.3204/PUBDB-2025-03912

Abstract: With industrial chemical processes facing the challenges of renewable energy supply, catalysts are needed that withstand fluctuations of operating conditions. For methanation reactions using hydrogen from electrocatalytic water splitting, dropouts of hydrogen are amongst the realistic scenarios. While Ni-based catalysts are the most widely used, bimetallic Ni/Fe-based catalysts recently emerged as superior. A new method of preparing highly active metallic catalysts is the decomposition of metal-organic frameworks. Even though it is difficult to control the particle size distribution and the homogeneity of the formed nanoparticles with this method, the carbonaceous features present between the nanoparticles permit avoiding the use of support, leading to a high-loading catalyst with superior stability. Here, we investigate with in situ X-ray absorption spectroscopy and pair distribution function analysis the structural details of a Ni3Fe@C methanation catalyst derived from a metal-organic framework during its activation and catalysis under H2-dropout conditions. Despite the similarity of these phases, it was possible to identify two fcc phases of Ni3Fe and Ni coexisting during catalytic cycling, with a Fe2NiO4 spinel phase appearing during dropouts. This indicates oxidation of the particle surface in the absence of hydrogen, which can be fully recovered by reactivation in pure hydrogen atmosphere, providing high stability of the catalyst during an industrially relevant dropout scenario.

Note: We acknowledge funding by the Deutsche Forschungsgemein-schaft (DFG, German Research Foundation) via SPP2080 (LU2246/3–1, BA 4467/8–1 and BA 4467/8–2, KL 2913/1–1 and KL2913/1–2, ZO 369/2–1 and ZO 369/2–2).

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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. FS-Proposal: I-20200879 (I-20200879) (I-20200879)

Experiment(s):

1. PETRA Beamline P65 (PETRA III)

Appears in the scientific report 2025

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Database coverage:
; ; ; Clarivate Analytics Master Journal List ; Current Contents - Physical, Chemical and Earth Sciences ; DEAL Wiley ; Ebsco Academic Search ; Essential Science Indicators ; IF < 5 ; JCR ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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