Mechanisms of Copper-Based Catalyst Deactivation during CO2 Reduction to Methanol

Despite the fact that the methanol synthesis process includes industrially some of the most important catalytic chemical reactions, it is still not clear how different gaseous species impact catalyst component structure. With the goal to reduce CO2 emissions through hydrogenation to CH3OH, a higher...

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Veröffentlicht in:Industrial & engineering chemistry research 2019-07, Vol.58 (29), p.13021-13029
Hauptverfasser: Prašnikar, Anže, Pavlišič, Andraž, Ruiz-Zepeda, Francisco, Kovač, Janez, Likozar, Blaž
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container_end_page 13029
container_issue 29
container_start_page 13021
container_title Industrial & engineering chemistry research
container_volume 58
creator Prašnikar, Anže
Pavlišič, Andraž
Ruiz-Zepeda, Francisco
Kovač, Janez
Likozar, Blaž
description Despite the fact that the methanol synthesis process includes industrially some of the most important catalytic chemical reactions, it is still not clear how different gaseous species impact catalyst component structure. With the goal to reduce CO2 emissions through hydrogenation to CH3OH, a higher H2O formation rate than in the production from compressed CO-rich feed should also be considered. It is known that steam accelerates the sintering of metals, several oxide compounds, and their interfaces. To determine the effect of moisture on the Cu/ZnO/Al2O3 catalysts, a commercial catalytic material was systematically aged at various gas compositions and analyzed using transient H2 surface adsorption, N2O pulse efficient chemisorption, X-ray photoelectron spectroscopy, scanning transmission electron microscopy mapping, X-ray powder diffraction, and N2 physisorption, and the mechanisms of deactivation were observed. A strong consistent relation between the compacting of Al2O3, the amount of water in the controlled streamflow, and the activity was found. This connected loss of support resulted in the (re)­forming of Cu, ZnO, and Cu/ZnO phases. Copper particle growth was modeled by applying a physical coalescence model. In the presence of CO and/or CH3OH, zinc oxide material started to cover the Cu granules, while H2O promoted the development of separate Cu regions.
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title Mechanisms of Copper-Based Catalyst Deactivation during CO2 Reduction to Methanol
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