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Ru and Re Doping Impact the Performance of MgxAlOy–SiO2 Catalysts in Ethanol Upgrading to 1; 3-Butadiene and 1-Butanol
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DOI：10.1021/acssuschemeng.6c03239.png)
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Abstract
En 中文
Beyond its established use as biofuel, ethanol upgrading into higher chemicals offers a viable route toward sustainable chemical production. The conversion of ethanol to 1,3-butadiene and 1-butanol involves an initial dehydrogenation step facilitated by dopant metals in acid–base catalysts. In this work, we investigated how incorporating low mass fractions (0.1 wt %) of Ru or Re into MgxAlOy–SiO2 catalysts influences their performance. Even at such low loadings, metal impregnation notably modified the catalysts’ physicochemical properties, leading to changes in conversion and selectivity. The metal-doped catalysts exhibited enhanced acetaldehyde selectivity (up to 39% for Ru), reflecting the promotion of ethanol dehydrogenation. However, the yield to condensation products remained modest, reaching a slight 5% increase for Ru relative to the undoped material. Overall, metallic sites favored ethanol dehydrogenation, while an appropriate basic-to-acid site ratio was crucial for the subsequent steps. Metal incorporation also reduced the total site density, particularly basic sites. The catalyst with Ru has a modest 6% higher density of acid sites compared to the number of basic sites, while the Re-doped material exhibits a pronounced 135% higher amount. Furthermore, both doped catalysts exhibited high structural and catalytic stability, as confirmed by operando X-ray diffraction and 70-h reaction tests.
Keywords:
Catalysts
Ethanol
Metals
Oxides
Selectivity
Ethanol upgrading
1,3-Butadiene
1-Butanol
Metal doping
Operando characterization
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