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000622772 1001_ $$0P:(DE-H253)PIP1093119$$aSchulte, Mariam L.$$b0
000622772 245__ $$aMonitoring the Fate of Zn in the Cu/ZnO/ZrO$_2$ Catalyst during CO$_2$‐to‐Methanol Synthesis at High Conversions by Operando Spectroscopy
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000622772 520__ $$aIn the frame of developing a sustainable chemical industry, heterogeneously catalyzed CO$_2$ hydrogenation to methanol has attracted considerable interest. However, the Cu-Zn based catalyst system employed in this process is very dynamic, especially in the presence of the products methanol and water. Deactivation needs to be prevented, but its origin and mechanism are hardly investigated at high conversion where product condensation is possible. Here, we report on the structural dynamics of a Cu/ZnO/ZrO$_2$ catalyst at 90 bar and 40% CO$_2$ conversion (at equilibrium conditions), investigated in a dedicated metal-based spectroscopic cell specially fabricated using additive manufacturing. This particular reactor configuration aims to mimic the high CO$_2$ conversion part of the catalyst bed and can induce product condensation, which is monitored by operando X-ray absorption spectroscopy. While Cu remained mostly stable throughout the experiment, Zn underwent strong restructuring. The chosen reaction conditions, including the use of CO$_2$ as carbon source and in situ product condensation, were selected to provide insights under industrial conditions. This work highlights the importance of spectroscopic investigations at high conversion levels, offering insights into chemical transformations during deactivation, extending the concept of spatially resolved studies, and thus providing guidance for the design of more stable catalysts.
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000622772 7001_ $$0P:(DE-H253)PIP1105191$$aTruttmann, Vera$$b1
000622772 7001_ $$0P:(DE-H253)PIP1017208$$aDoronkin, Dmitry E.$$b2
000622772 7001_ $$0P:(DE-H253)PIP1100120$$aBaumgarten, Lorena$$b3
000622772 7001_ $$0P:(DE-H253)PIP1107811$$aNicolai, Alexander$$b4
000622772 7001_ $$aBeltran, Diego Alejandro Montalvo$$b5
000622772 7001_ $$aSumm, Florian J.$$b6
000622772 7001_ $$aKiener, Christoph$$b7
000622772 7001_ $$aWarmuth, Lucas$$b8
000622772 7001_ $$aPitter, Stephan$$b9
000622772 7001_ $$0P:(DE-H253)PIP1097957$$aSaraçi, Erisa$$b10
000622772 7001_ $$0P:(DE-H253)PIP1008522$$aGrunwaldt, Jan-Dierk$$b11$$eCorresponding author
000622772 773__ $$0PERI:(DE-600)2011836-3$$a10.1002/anie.202423281$$gp. e202423281$$n15$$pe202423281$$tAngewandte Chemie / International edition$$v64$$x1433-7851$$y2025
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