Effect of Iron Oxide Modification on the Catalytic Properties of Pd/ZrSBA-15 in Reductive Dichlorination of Diclofenac

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Abstract

Palladium (0.1 wt %) or palladium together with iron (0.2 and 11.7 wt %) was applied by wet impregnation onto ordered mesoporous material of SBA-15 type, including silicon and zirconium oxides. The obtained catalysts were tested in hydrodechlorination of microoctoxicant diclofenac in aqueous solution (150 mg/L) in batch reactor at 30°C in hydrogen atmosphere after reduction at 30 or 320°C with hydrogen. Addition of iron and reduction under mild conditions contributed to increase of catalyst activity. High ability of palladium to reduction under mild conditions in such catalysts was revealed by X-ray photoelectron spectroscopy method, and addition of iron slightly decreases Pd0/(Pd0 + Pd2+) ratio on surface. Iron is present in the catalyst in the form of FeO and Fe3O4 oxides; after reduction at 320°C FeO predominates on the surface, while after reduction at 30°C predominating form is Fe3O4. According to transmission electron microscopy and X-ray diffraction data, the dispersion of palladium is somewhat higher in the iron-containing catalyst. The results of temperature-programmed reduction and infrared diffuse reflectance spectroscopy of adsorbed CO indicate a strong interaction of palladium with iron oxides with the formation of new types of active centers.

About the authors

E. S. Lokteva

Lomonosov Moscow State University

Email: LES@kge.msu.ru
Moscow, Russia

E. G. Khachatryan

Lomonosov Moscow State University

Moscow, Russia

M. D. Pesotsky

Lomonosov Moscow State University

Moscow, Russia

K. I. Maslakov

Lomonosov Moscow State University

Moscow, Russia

S. V. Maksimov

Lomonosov Moscow State University

Moscow, Russia

A. N. Kharlanov

Lomonosov Moscow State University

Moscow, Russia

E. V. Golubina

Lomonosov Moscow State University

Moscow, Russia

I. Yu. Kaplin

Lomonosov Moscow State University

Moscow, Russia

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