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Jakobsen, Helene Hagemann
in Cooperation with on an Cooperation-Score of 37%
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Publications (3/3 displayed)
- 2024Using CoCu2Ga/SiO2 to identify stability-issues in ethanol-selective Co-Cu alloyed catalysts in carbon monoxide hydrogenationcitations
- 2024Using CoCu 2 Ga/SiO 2 to identify stability-issues in ethanol-selective Co-Cu alloyed catalysts in carbon monoxide hydrogenationcitations
- 2024Using CoCu$_2$Ga/SiO$_2$ to identify stability-issues in ethanol-selective Co-Cu alloyed catalysts in carbon monoxide hydrogenation
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article
Using CoCu2Ga/SiO2 to identify stability-issues in ethanol-selective Co-Cu alloyed catalysts in carbon monoxide hydrogenation
Abstract
<p>Hydrogenation of CO to higher alcohols such as ethanol is an attractive pathway for industrial production while avoiding competition with food crops. However, thermocatalytic ethanol production from syngas is currently hindered by the lack of selective catalysts. The structural integrity of ternary-alloyed CoCu<sub>2</sub>Ga nanoparticles supported on silica was studied during thermo-catalytic CO hydrogenation. Catalysts of four different CoCu<sub>2</sub>Ga weight-loadings were tested catalytically under differential conversion, showing their different intrinsic selectivity during CO hydrogenation towards ethanol, methanol, and hydrocarbons. CoCu<sub>2</sub>Ga catalysts with 3.5 wt% and 17.8 wt% proved most and least selective towards ethanol formation, respectively. These two were studied in depth using STEM-EDX of fresh and spent samples showing different size distributions of the nanoparticles for all samples, and a change in the Co/Cu distribution of the nanoparticles from fresh to spent samples. In situ characterization using XRD, XANES, and EXAFS during CO hydrogenation supported the findings of the STEM-EDX and elucidated that the fresh more homogenous catalyst consisting of ternary CoCu<sub>2</sub>Ga nanoparticles de-alloyed into Cu-rich and CoGa-rich nanoparticles. This de-alloying was possibly driven by two factors: the metastable phase of CoCu<sub>2</sub>Ga decreasing its free energy by separating Cu and Co; and the strong interaction between Co and CO further driving a segregation. From a theoretical standpoint, Cu-Co intermetallics present the most selective catalyst to form ethanol over methane and methanol. The experimental findings presented here support the theory, although further efforts are needed to improve structural stability during the catalytic reaction.</p>