Pd Nanoparticles Immobilized on Pyridinic N-Rich Carbon Nanosheets for Promoting Suzuki Cross-Coupling Reactions.

Abstract

Palladium (Pd) catalysts play a crucial role in facilitating Suzuki cross-coupling reactions for the synthesis of valuable organic compounds. However, conventional heterogeneous Pd catalysts often encounter challenges such as leaching and deactivation during reactions, leading to reduced catalytic efficiency. In this study, we employed an innovative intercalation templating strategy to prepare two-dimensional carbon nanosheets with high nitrogen doping derived from petroleum asphalt, which were utilized as a versatile support for immobilizing Pd nanoparticles (Pd/N-CNS) in efficient Suzuki cross-coupling reactions. The results indicate that the anchoring effect of high-pyridinic N species on the two-dimensional carbon nanosheets enhances interactions between Pd and the support, effectively improving both the dispersibility and stability of the Pd nanoparticles. Notably, the Pd/N-CNS catalyst achieved an overall turnover frequency (TOF) of 2390 h^-1 for the Suzuki cross-coupling reaction under mild conditions, representing approximately a nine-fold increase in activity compared to commercial Pd/C catalysts. Furthermore, this catalyst maintained an overall TOF of 2294 h^-1 even after five reaction cycles, demonstrating excellent stability. Theoretical calculations corroborate these observed enhancements in catalytic performance by attributing them to improved electron transfer from Pd to the support facilitated by abundant pyridinic N species. This work provides valuable insights into feasible strategies for developing efficient catalysts aimed at sustainable production of biaromatic compounds.