COx-free H2, along with uniform carbon nanotubes, can be achieved together in high yield by CH4 decomposition. It only needs a proper catalyst and reaction condition. Herein, Fe-based catalyst dispersed over titania-incorporated-alumina (Fe/Ti-Al), with the promotional addition of lanthanides, like CeO2 and La2O3, over it, is investigated for a methane decomposition reaction at 800 °C with GHSV 6 L/(g·h) in a fixed-bed reactor. The catalysts are characterized by temperature-programmed reduction (TPR), powder X-ray diffraction (XRD), Raman spectroscopy, and transmission electron microscopy (TEM). The promoted catalysts are facilitated with higher surface area and enhanced dispersion and concentration of active sites, resulting in higher H2 and carbon yields than unpromoted catalysts. Ceria-promoted 20Fe/Ti-Al catalyst had the highest concentration of active sites and always attained the highest activity in the initial hours. The 20Fe-2.5Ce/Ti-Al catalyst attains >90% CH4 conversion, >80% H2-yield, and 92% carbon yield up to 480 min time on stream. The carbon nanotube over this catalyst is highly uniform, consistent, and has the highest degree of crystallinity. The supremacy of ceria-promoted catalyst attained >90% CH4 conversion even after the second cycle of regeneration studies (against 87% in lanthanum-promoted catalyst), up to 240 min time on stream. This study plots the path of achieving catalytic and carbon excellence over Fe-based catalysts through CH4 decomposition.
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