Synthesis and catalytic properties of nitrogen-containing carbon nanotubes

Abstract

Nitrogen-containing carbon nanotubes (CNTs) were synthesized by the CVD method on oxide catalysts of Al-Fe-Mo-O by adding acetonitrile or ethylenediamine to the carbon source (propylene), or completely replacing it, as well as impregnating the original CNTs with urea, followed by heat treatment. The structure of nitrogen-containing CNTs (N-CNT) was characterized by the method of Raman scattering, transmission electron microscopy (TEM), differential thermal and gravimetric analysis (DTA, DTG) and X-ray photoelectron spectroscopy (XPS). The influence of the synthesis method on the number and chemical state of nitrogen heteroatoms in the structure of the carbon matrix is found. According to the TEM, nitrogen-containing CNTs have a characteristic bamboo-like structure, which is less perfect compared to the structure of the original CNTs: the characteristic Raman bands (G and D) are shifted to higher frequencies, their half-width and band D intensity increase relative to G. This is also manifested in the lower thermal stability of nitrogen-containing CNTs. According to the XPS, the direct synthesis of nitrogen-containing CNTs increases the total content of nitrogen atoms and the proportion of pyrrolic and quaternary nitrogen against the background of a significant decrease in the amount of pyridinic form. This can be explained by the fact that nitrogen is evenly distributed throughout the carbon matrix of CNTs, and during nitriding of CNTs with urea, nitrogen is included mainly in the surface layers and defects, because the pyridine form is characteristic of the edge location of the nitrogen atom in the graphene plane.The catalytic effect of multilayer nitrogen-containing carbon nanotubes (N-CNT) on the kinetics of decomposition of hydrogen peroxide in aqueous solutions at different pH values is considered. It is concluded that the method of direct synthesis of nitrogen-containing CNTs allows to obtain more catalytically active carbon nanotubes containing more nitrogen, mainly pyrrolic and quaternary type. It has been found that regardless of the method of synthesis, the maximum catalytic activity in the decomposition of hydrogen peroxide is observed at pH 7.