Journal Article

PUBDB-2025-00466

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Monitoring the Fate of Zn in the Cu/ZnO/ZrO$_2$ Catalyst during CO$_2$‐to‐Methanol Synthesis at High Conversions by Operando Spectroscopy

Schulte, M. L.Extern* ; Truttmann, V.Extern* ; Doronkin, D. E.Extern* ; Baumgarten, L.Extern* ; Nicolai, A.Extern* ; Beltran, D. A. M. ; Summ, F. J. ; Kiener, C. ; Warmuth, L. ; Pitter, S. ; Saraçi, E.Extern* ; Grunwaldt, J.-D. (Corresponding author)Extern*

2025
Wiley-VCH Weinheim

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Please use a persistent id in citations: doi:10.1002/anie.202423281  doi:10.3204/PUBDB-2025-00466

Abstract: In the frame of developing a sustainable chemical industry, heterogeneously catalyzed CO$_2$ hydrogenation to methanol has attracted considerable interest. However, the Cu-Zn based catalyst system employed in this process is very dynamic, especially in the presence of the products methanol and water. Deactivation needs to be prevented, but its origin and mechanism are hardly investigated at high conversion where product condensation is possible. Here, we report on the structural dynamics of a Cu/ZnO/ZrO$_2$ catalyst at 90 bar and 40% CO$_2$ conversion (at equilibrium conditions), investigated in a dedicated metal-based spectroscopic cell specially fabricated using additive manufacturing. This particular reactor configuration aims to mimic the high CO$_2$ conversion part of the catalyst bed and can induce product condensation, which is monitored by operando X-ray absorption spectroscopy. While Cu remained mostly stable throughout the experiment, Zn underwent strong restructuring. The chosen reaction conditions, including the use of CO$_2$ as carbon source and in situ product condensation, were selected to provide insights under industrial conditions. This work highlights the importance of spectroscopic investigations at high conversion levels, offering insights into chemical transformations during deactivation, extending the concept of spatially resolved studies, and thus providing guidance for the design of more stable catalysts.

Note: Supposed to be Open Access covered by Project Deal (after corresponding author signs the publishing agreement).

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Contributing Institute(s):

1. FS DOOR-User (FS DOOR-User)

Research Program(s):

1. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
2. FS-Proposal: I-20230260 (I-20230260) (I-20230260)
3. DFG project G:(GEPRIS)460248799 - DAPHNE4NFDI - DAten aus PHoton- und Neutronen Experimenten für NFDI (460248799) (460248799)

Experiment(s):

1. PETRA Beamline P65 (PETRA III)

Appears in the scientific report 2025

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Database coverage:
; ; ; Chemical Reactions ; Clarivate Analytics Master Journal List ; Current Contents - Life Sciences ; Current Contents - Physical, Chemical and Earth Sciences ; DEAL Wiley ; Ebsco Academic Search ; Essential Science Indicators ; IF >= 15 ; Index Chemicus ; JCR ; Nationallizenz ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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