Evaluation of highly active and stable SiO2 supported Fe-based catalysts for the catalytic methane decomposition into COx free hydrogen and CNTs

Abstract

Catalytic methane decomposition is believed to be an economic and environmental friendly route for the production of COx free hydrogen and high quality carbon nanotubes. However, the development of active and stable catalysts remains a significantly challenging research topic. This study focuses on the development of highly active and stable silica-supported Fe-based catalysts for the thermal decomposition of methane into hydrogen and high quality carbon nanotubes. A series of Fe/SiO2 catalysts with varying Fe loading in the range between 25 wt% and 100 wt% were synthesized by the solution combustion synthesis (SCS) method. The synthesized catalysts were characterized by various bulk sensitive and surface sensitive analytical tools, such as SEM, XRD, HRTEM, BET and Raman spectroscopy. All supported catalysts exhibited comparatively high activity than the unsupported 100 wt% Fe (denoted as 100F) catalyst which was the least active. Moreover, the catalytic activity in terms of methane conversion, methane decomposition rate, growth activities as well as carbon yields increased with an increase in the Fe loading. At an operating temperature of 650 °C and a GHSV of 8000 h−1, the 75FS catalyst, with a composition of 75 wt%Fe/SiO2, demonstrated the highest methane decomposition rate of 0.75gCH4/g-cat.h among the investigated catalysts. Additionally, after achieving initial stability at about 120 min, this catalyst remained active throughout testing on stream for 900 min. TEM and SEM analysis of the spent catalyst showed that the supported 75FS catalyst produced multi-walled carbon nanotubes with uniform diameters of 28 nm and with Id/Ig ratio of 0.454 whereas the unsupported 100F catalyst mainly produced graphene sheets.