Tuning of nitrogen-doped carbon nanotubes as catalyst support for liquid-phase reaction

Abstract

This work reports the synthesis of nitrogen-doped carbon nanotubes (N-CNTs) using a Chemical Vapor Deposition (CVD) process at temperature ranging from 600 °C to 850 °C and ethane/ammonia concentration (defined as a volume percentage of C 2H 6/(C 2H 6 + NH 3)) of 20–100%. Several characterizations, i.e. XPS, SEM and TEM were done on the as-synthesized nitrogen-doped carbon nanotubes in order to get more insight about the influence of the synthesis conditions on the characteristics and properties of these N-CNTs. Depending on the synthesis conditions, the atomic percentage of nitrogen in carbon nanotubes varied from 0 at.% to about 5.5 at.%. The undoped carbon nanotubes (N-free CNTs) and two kinds of N-CNTs with different types of nitrogen incorporated species have been used as the supports for palladium in the liquid-phase hydrogenation of cinnamaldehyde. The introduction of nitrogen atoms into the carbon matrix significantly modified the chemical properties of the support compared to the N-free carbon nanotube resulting in a higher metal dispersion. N-CNTs exhibit much higher activity in the hydrogenation reaction compare to the undoped ones. Nitrogen incorporation also strongly improved the selectivity towards the C C bond hydrogenation. The results show that the type of nitrogen species incorporated in CNTs structure can also influence the catalytic activity. Recycling test confirms the high stability of the catalyst as neither palladium leaching nor deactivation has been observed.