Pd Nanoparticles Supported on Amine-Functionalized MgAl Layered Double Hydroxides for Solvent-Free Aerobic Oxidation of Benzyl Alcohol

Abstract

Pd nanoparticles (NPs) supported on amine-functionalized layered double hydroxides (LDHs) (Pd/NH2-LDH-NS) were successfully obtained by implanting aminopropyltriethoxysilane (APTS) on MgAl LDH nanosheets (LDH-NS), followed by impregnating [Pd(NH3)4]Cl2 and reduction with NaBH4. The physicochemical characteristics of the obtained Pd/NH2-LDH-NS were characterized by X-ray diffraction (XRD), Fourier transform infrared (FT-IR),, N2 adsorption–desorption, inductive coupled plasma (ICP), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy(XPS), and their catalytic performance was tested in the selective oxidation of benzyl alcohol with molecular oxygen under solvent-free and base-free conditions. The results showed that the implanted –NH2 groups can promote the dispersion of the supported Pd NPs via complexation of the implanted –NH2 groups to Pd NPs, and they can increase the surface basicity of the catalysts, thus enhancing the catalytic activity and selectivity to benzylaldehyde. Pd/NH2-LDH-NS exhibited enhanced catalytic activity (31.6%) and selectivity (>98%) compared to the corresponding Pd/LDH-NS, Pd/LDH, Pd/SiO2, and Pd/Al2O3. Moreover, Pd/NH2-LDH-NS was remarkably stable and could be reused at least four times without a significant loss in activity and selectivity.