Formation of carbon nanotubes on iron/cobalt oxides supported on zeolite-Y: Effect of zeolite textural properties and particle morphology

Abstract

The effect of the textural properties and morphology of zeolite Y, used as support of iron (Fe) or cobalt (Co) oxides, on the quantity and quality of the multi-wall carbon nanotubes (MWNTs) synthesized by catalytic chemical vapour deposition (CCVD) of acetylene was studied. The parent zeolite Y was modified by various dealumination procedures, namely hydrothermal treatment (steaming), treatment with ammonium hexafluorosilicate (AHFS) and combined steaming-AHFS. The ion-exchange and wet impregnation methods were used for supporting the metals on the zeolite Y samples, with the latter method providing the most effective catalysts for carbon nanotube (CNT) formation. Severe dealumination of zeolite-Y by steaming, which induced the formation of secondary meso/macropores and of relatively large particles/aggregates, resulted in significant decrease in the formation of CNTs compared to the catalysts based on the parent zeolite-Y. Post-treatment of the steamed samples with AHFS had no beneficial effect on the catalysts’ activity. Moderate dealumination of the parent zeolite Y by AHFS also inhibited the formation of CNTs, but to a lesser extent compared to the catalysts based on steamed zeolite Y. The TGA studies revealed the presence of carbon phases with different thermal stability in the zeolite–CNT composites, ranging from amorphous carbon to well-graphitized MWNTs. TEM images and micro-Raman spectra taken right after growth confirmed the formation of high quality MWNTs with a low degree of disorder irrespective of the catalysts used, the degree of dealumination of the zeolite Y and the textural and morphological characteristics of the zeolitic support.