Autor: |
Shishova, V. V., Lokteva, E. S., Maksimov, G. S., Maslakov, K. I., Kaplin, I. Yu., Maksimov, S. V., Golubina, E. V. |
Zdroj: |
Moscow University Chemistry Bulletin; Jun2024, Vol. 79 Issue 3, p156-169, 14p |
Abstrakt: |
Pd/ZrO2 and Pd/ZrO2SiO2 catalysts prepared by wet impregnation and reduced with H2 under mild (30°C, aqueous suspension) or harsh (320°C) conditions are compared in the hydrodechlorination of the microecotoxicant diclofenac (DCF) in an aqueous solution at 30°С. According to the TPR and XPS data, the addition of SiO2 to the support reduces the degree of metal-support interaction and facilitates the reduction of palladium. Despite the lower Pd0 fraction, the Pd/ZrO2 catalyst is more active in the batch reactor: after reduction at 320°С, it slightly, and after mild reduction, significantly (7 times), exceeds Pd/ZrO2SiO2 in catalytic activity. XRD and TEM show a wider size distribution of palladium nanoparticles in the Pd/ZrO2 sample, while low-temperature N2 adsorption, XPS, and TPR demonstrated better accessibility of palladium on the Pd/ZrO2 surface due to the reduced decoration by the support components and increased pore size. These features explain the increased activity of Pd/ZrO2. Testing in the flow system demonstrated higher DCF conversion in the presence of catalysts reduced at 320°C and higher stability of Pd/ZrO2SiO2 compared to Pd/ZrO2. The stability is ensured by the increased reducibility of Pd2+ with H2 and by the developed surface of Pd/ZrO2SiO2, which prevents deactivation under the action of HCl released in hydrodechlorination. [ABSTRACT FROM AUTHOR] |
Databáze: |
Complementary Index |
Externí odkaz: |
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