2020
DOI: 10.1002/cctc.202000777
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Cu−Zn Alloy Formation as Unfavored State for Efficient Methanol Catalysts

Abstract: The active sites of Cu/ZnO‐based catalysts, commercially applied for the hydrogenation of CO2 or CO2‐rich synthesis gas, are still subject of current debates. Generally, the discussion is focused on the nature of the interfacial contact between Cu and ZnO, particularly whether it is rather of oxidic (Cu−ZnO) or alloying (Cu−Zn) character. We report on kinetic investigations on a Cu/ZnO : Al high performance catalyst activated at different temperatures. Incrementally increasing temperature under reductive condi… Show more

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Cited by 48 publications
(111 citation statements)
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“…XAS revealed the absence of palladium-zinc de-alloying or any indication of the surface oxidation of palladium, which might be expected due to possible palladium-formate intermediates,d uring the catalytic cycle.I nstead, transient experiments show that the palladium-zinc phase is very stable under different gas atmospheres (hydrogen, CO 2 /H 2 mixture and carbon dioxide) and it may well be only responsible for hydrogen activation, while carbon dioxide activation, and its subsequent hydrogenation, occur on the zinc oxide similar to the Cu/ZnObased system. [25,26] However,a tt his point, it is not clear, whether the palladium-zinc alloy alone governs the activity and selectivity of the catalyst, or the interface between the alloy phase and bulk zinc oxide represents the active site for the selective transformation of carbon dioxide to methanol.…”
Section: Resultsmentioning
confidence: 99%
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“…XAS revealed the absence of palladium-zinc de-alloying or any indication of the surface oxidation of palladium, which might be expected due to possible palladium-formate intermediates,d uring the catalytic cycle.I nstead, transient experiments show that the palladium-zinc phase is very stable under different gas atmospheres (hydrogen, CO 2 /H 2 mixture and carbon dioxide) and it may well be only responsible for hydrogen activation, while carbon dioxide activation, and its subsequent hydrogenation, occur on the zinc oxide similar to the Cu/ZnObased system. [25,26] However,a tt his point, it is not clear, whether the palladium-zinc alloy alone governs the activity and selectivity of the catalyst, or the interface between the alloy phase and bulk zinc oxide represents the active site for the selective transformation of carbon dioxide to methanol.…”
Section: Resultsmentioning
confidence: 99%
“…Instead, transient experiments show that the palladium-zinc phase is very stable under different gas atmospheres (hydrogen, CO2/H2 mixture and carbon dioxide) and it may well be only responsible for hydrogen activation, while carbon dioxide activation, and its subsequent hydrogenation, occur on the zinc oxide similar to the Cu/ZnObased system. [27,28] However, at this point, it is not clear, whether 10.1002/anie.202103087…”
Section: Accepted Manuscriptmentioning
confidence: 99%
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“…Taking into account recent works, [25–28] which have questioned the role of copper‐zinc alloy in methanol synthesis from carbon dioxide, an operando investigation of carbon dioxide hydrogenation over Pd/ZnO system is warranted to understand the true nature of the active sites and to verify the role that a palladium–zinc alloy phase may have in facilitating this reaction. We therefore report a combined high‐pressure operando study of methanol synthesis over Pd/ZnO catalysts using XAS, XRD and FTIR techniques.…”
Section: Introductionmentioning
confidence: 99%