Preparation of core-shell catalyst for the tandem reaction of amino compounds with aldehydes.

Abstract

Heterogeneous noble metal-based catalysts with stable, precise structures and high catalytic performance are of great research interest for sustainable catalysis. In this article, we designed a novel core-shell catalyst, Pd@UiO-66-NH2@mSiO2, with Pd@UiO-66-NH2 as the core and mesoporous SiO2 (mSiO2) as the shell. Scanning electron microscopy (SEM), X-ray diffraction (XRD) and Fourier transform infrared spectroscopy (FT-IR) measurement results demonstrated that the obtained catalyst has an excellent core-shell structure. It can significantly prevent the aggregation of Pd nanoparticles (NPs), as well as the leaching of Pd NPs during the reaction process, owing to the protective effect of mSiO2. During the tandem reaction of aniline and benzaldehyde to generate secondary amines, the prepared Pd@UiO-66-NH2@mSiO2 is highly efficient, due to the strong acid sites provided by UiO-66-NH2 and the hydrogenation reduction sites provided by Pd NPs. Meanwhile, the Pd@UiO-66-NH2@mSiO2 with porous structure can also enhance the mass transfer of reactants to improve the reaction efficiency. Additionally, the prepared catalyst was used to catalyze the series reaction of amino compounds and aldehydes, and the results showed that just 5 mg of the catalyst can convert more than 99% of the reactants within 60 minutes in the presence of 1 atm H2 at room temperature. Finally, the selectivity and stability of the as-prepared catalyst were also confirmed.