Highly Dispersed Pd Nanoparticles Supported on Zr-Doped MgAl Mixed Metal Oxides for 2-Ethylanthraquinone Hydrogenation

Abstract

In this study, Pd-Mg(Al)-LDH/γ-Al₂O₃ and Pd-Mg(Al)Zr-LDH/γ-Al₂O₃ precursors were synthesized by impregnating Na₂PdCl₄ on Mg(Al)-LDH/γ-Al₂O₃ and Mg(Al)Zr-LDH/γ-Al₂O₃, and then the precursors were calcinated and reduced to obtain Pd-Mg(Al)-MMO/γ-Al₂O₃ and Pd-Mg(Al)Zr-MMO/γ-Al₂O₃ catalysts. Compared with Pd/γ-Al₂O₃ catalyst, the hydrogenation efficiency of Pd-Mg(Al)-MMO/γ-Al₂O₃ and Pd-Mg(Al)Zr-MMO/γ-Al₂O₃ increased by 15.7% and 24.0%, respectively. Moreover, the stability of Pd-Mg(Al)Zr-MMO/γ-Al₂O₃ catalyst was also higher than that of Pd/γ-Al₂O₃. After four runs, the hydrogenation efficiency of Pd/γ-Al₂O₃ decreased from 12.1 to 10.0 g/L, while that of Pd-Mg(Al)Zr-MMO/γ-Al₂O₃ decreased from 15.0 to 14.3 g/L. The active aquinones selectivities of all catalysts were almost 99%. The structures of the catalysts were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), N₂ adsorption–desorption, inductively coupled plasma-atomic emission spectrometry (ICP-AES), CO chemisorption analysis, transmission electron microscopy (TEM), temperature-programmed reduction with hydrogen (H₂-TPR), and X-ray photoelectron spectroscopy (XPS). The results indicate that the improved catalytic performance is attributed to the stronger interaction between Pd and Mg(Al)Zr-MMO/γ-Al₂O₃, smaller Pd particle size and higher Pd dispersion. This work develops an effective method to synthesize highly dispersed Pd nanoparticles based on the layered double hydroxides (LDHs) precursor.

Keywords

LDHs precursor / Mixed metal oxides / Pd nanoparticles / 2-Ethylanthraquinone hydrogenation / Hydrogen peroxide

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