Carbon nanotubes production from catalytic pyrolysis of polyethylene over nickel-based catalysts: The influence of support materials

Abstract

To understand the influence of support materials on the reactivity of catalysts, four nickel- based catalysts supported on different materials (ZrO2, TiO2, Nb2O5, and Al2O3) were developed and investigated in the carbon nanotubes production from catalytic pyrolysis of polyethylene using two-stage fixed bed reactor. The results showed that the Ni/Al2O3 catalyst generated the highest carbon material yield of 36.5 wt%, while the order of carbon material yield was Ni/Al2O3 > Ni/TiO2 > Ni/ZrO2 > Ni/Nb2O5. To explore the correlation between catalysts properties and carbon products, the essential structural characteristics of fresh catalyst and reacted catalyst were analyzed by powder X-ray diffraction (XRD), scanning electron microscopy (SEM), high resolution transmission electron microscopy (TEM), temperature program oxidation (TPO), nitrogen adsorption measurements and Raman spectroscopy. The Ni/Al2O3 catalyst with the highest surface area, abundant pore structure, and moderate metal-support interaction promoted the decomposition of pyrolysis volatiles to produce carbon nanomaterials, which were consist of carbon nanotubes (CNTs). CNTs are the main component of carbon materials produced, accounting for a relatively high proportion. In comparison, the large metal active particles and weak metal-support interaction of Ni/TiO2 catalyst had a negative impact on the formation of CNTs, generating many fishbone like carbon nanofibers (CNFs). Moreover, the poor pore structure and larger metal active particles for Ni/ZrO2 and Ni/Nb2O5 catalyst led to a low carbon deposition yield and poor quality of CNTs. The results provide valuable data and theoretical support for the research on the preparation of valuable carbon nanotubes from waste plastics.