Three-dimensional N-doped graphene aerogel-supported Pd nanoparticles as efficient catalysts for solvent-free oxidation of benzyl alcohol.

Abstract

Herein, three-dimensional (3D) nitrogen-doped graphene with large surface areas and abundant porous structures was prepared by a hydrothermal synthesis method, which served as a novel support to enhance the catalytic properties of noble metal catalysts for the solvent-free selective oxidation of benzyl alcohol. The as-prepared samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, Fourier transform infrared (FTIR) spectroscopy, and Brunauer–Emmett–Teller (BET) method. The results clearly showed that the introduced N-containing group prevented the aggregation of graphene sheets and provided more structural defects to maximize the number of exposed active sites. The three-dimensional structure can provide a unique porous structure and large specific surface area. Moreover, the three-dimensional structure makes the recycling and reuse of the catalyst easier. The combination of these properties results in the reduction of the average particle size of metal palladium to 3.2 nm; this significantly increases the catalytic activity of the catalyst. The three-dimensional N-doped graphene aerogel-supported Pd nanoparticle (3D Pd/NRGO) composites exhibit excellent catalytic activity for the solvent-free selective oxidation of benzyl alcohol to benzaldehyde by molecular oxygen at 90 °C for 3 hours under atmospheric pressure, resulting in a 72.2% conversion of benzyl alcohol with 94.5% selectivity for benzaldehyde. In addition, the catalytic efficiency shows no obvious loss even after six repeated cycles. Thus, 3D Pd/NRGO can be used as an efficient, easily separable, recyclable, and stable catalyst for the solvent-free selective oxidation of benzyl alcohol under relatively mild conditions.