Journal Article

PUBDB-2021-02551

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Photo-Chemically-Deposited and Industrial Cu/ZnO/Al$_{2}$O$_{3}$ Catalyst Material Surface Structures During CO$_{2}$ Hydrogenation to Methanol: EXAFS, XANES and XPS Analyses of Phases After Oxidation, Reduction, and Reaction

Pori, M. ; Arčon, I.Extern* ; Dasireddy, V. D. B. C. ; Likozar, B. ; Orel, Z. C. ; Marinšek, M. (Corresponding author)

2021
Springer Science + Business Media B.V Dordrecht [u.a.]

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Please use a persistent id in citations: doi:10.1007/s10562-021-03556-1

Abstract: Industrial Cu/ZnO/Al$_2$O$_3$ or novel rate catalysts, prepared with a photochemical deposition method, were studied under functional CH$_3$OH synthesis conditions at the set temperature (T) range of 240–350 °C, 20 bar pressure, and stoichiometric carbon dioxide/hydrogen composition. Analytical scanning electron microscopy (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), X-ray adsorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) methods were systematically utilized to investigate the interfaces, measured local geometry, and chemical state electronics around the structured active sites of commercially available Cu/ZnO/Al$_2$O$_3$ material or synthesized Cu/ZnO. Processed Cu K-edge EXAFS analysis suggested that various Cu atom species, clusters, metallic fcc Cu, Cu oxides (Cu$_2$O or CuO) and the Cu$_{0.7}$Zn$_2$ alloy with hexagonal crystalline particles are contained after testing. It was proposed that in addition to the model’s Cu surface area, the amount, ratio and dispersion of the mentioned bonded Cu compounds significantly influenced activity. Additionally, XPS revealed that carbon may be deposited on the commercial Cu/ZnO/Al$_2$O$_3$, forming the inactive carbide coating with Cu or/and Zn, which may be the cause of basicity’s severe deactivation during reactions. The selectivity to methanol decreased with increasing T, whereas more Cu$_{0.7}$Zn$_2$ inhibited the CO formation through reverse water–gas shift (RWGS) CO$_2$ reduction.

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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-20160764 EC (I-20160764-EC) (I-20160764-EC)

Experiment(s):

1. PETRA Beamline P64 (PETRA III)

Appears in the scientific report 2021

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

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