Pd and Pd–CuO nanoparticles in hollow silicalite-1 single crystals for enhancing selectivity and activity for the Suzuki–Miyaura reaction

Abstract

Pd and Pd–CuO nanoparticles were successfully encapsulated in hollow silicalite-1 single crystals by tetrapropylammonium hydroxide (TPAOH) hydrothermal treatment with an “impregnation-dissolution-recrystallization” process. The size and number of particles in the hollow zeolite depended mainly on the nature of the metal. For palladium, the palladium nanoparticles easily aggregated into larger particles in the hydrothermal process, which displays excellent substrate selectivity for the meta- and para-substituted aryl bromides in the Suzuki–Miyaura reaction. For Pd–CuO binary metals (oxide), introducing copper oxide prevents aggregation of palladium, which shows about 3 times higher activity than encapsulated single Pd catalyst for the above reaction. The strategy using a hollow zeolite crystal as a support is a more reliable method for preparing multi-metallic (oxide) catalysts with well-dispersed nanoparticles.