Sonochemical Deposition of Palladium Nanoparticles Onto the Surface of N-Doped Carbon Nanotubes: A Simplified One-Step Catalyst Production Method

Abstract

Abstract: This work presents an easy, one-step procedure for catalyst preparation. A small fraction of palladium ions was reduced to Pd nanoparticles and deposited onto the surface of nitrogen-doped carbon nanotubes (N-BCNT) by acoustic cavitation using high-intensity ultrasound in aqueous phase, where N-BCNT served as a reducing agent. The formation of elemental palladium and palladium oxides were confirmed and the particle size is < 5 nm. The catalytic activity of the synthesized Pd/N-BCNT catalyst was tested in nitrobenzene hydrogenation at four different temperature (273–323 K) and 20 bar pressure. The catalyst showed high activity despite the presence of palladium oxide forms, the conversion of nitrobenzene to aniline was 98% at 323 K temperature after 40 min. The activation energy was 35.81 kJ/mol. At 303 K and 323 K temperature, N-methylaniline was formed as by-product in a small quantity (8 mmol/dm3). By decreasing the reaction temperature (at 273 K and 283 K), the reaction rate was also lower, but it was favourable for aniline selectivity, and not formed n-methylaniline. All in all, Pd/N-BCNT catalyst was successfully produced by using a one-step sonochemical method, where further activation was not necessary as the catalytic system was applicable in nitrobenzene hydrogenation. Graphic Abstract: [Figure not available: see fulltext.].