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Hydrodechlorination of Diclofenac in an Aqueous Solution over Pd/ZrO2 and Pd/ZrO2SiO2 Catalysts

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Moscow University Chemistry Bulletin Aims and scope

Abstract

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.

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ACKNOWLEDGMENTS

The authors acknowledge the support they received from the Moscow State University Program of Development.

Funding

This study was carried out as part of state assignment no. AAAAA21-121011990019-4 “Physical chemistry of the surface, adsorption and catalysis.”

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Authors and Affiliations

  1. Department of Chemistry, Moscow State University, 119991, Moscow, Russia

    V. V. Shishova, E. S. Lokteva, G. S. Maksimov, K. I. Maslakov, I. Yu. Kaplin, S. V. Maksimov & E. V. Golubina

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  1. V. V. Shishova
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  2. E. S. Lokteva
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  3. G. S. Maksimov
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  4. K. I. Maslakov
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  5. I. Yu. Kaplin
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  6. S. V. Maksimov
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  7. E. V. Golubina
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Correspondence to E. S. Lokteva.

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Translated by Sh. Galyaltdinov

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Shishova, V.V., Lokteva, E.S., Maksimov, G.S. et al. Hydrodechlorination of Diclofenac in an Aqueous Solution over Pd/ZrO2 and Pd/ZrO2SiO2 Catalysts. Moscow Univ. Chem. Bull. 79, 156–169 (2024). https://doi.org/10.3103/S0027131424700123

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