ARTICLE
This journal isThe catalytic stabilities of Fe-modified and -unmodified 5%Mo/HZSM-5 catalysts in the non-oxidative methane dehydroaromatization were compared at 1073 K and three reaction/H 2 -regeneration cycle periods: 5 min CH 4 -5 min H 2 , 5 min CH 4 -10 min H 2 , and 5 min CH 4 -20 min H 2 . Fe addition proved capable of remarkably increasing the catalyst stability over the cycles of 5 min CH 4 -20 min H 2 but hardly effective over the cycles of 5 min CH 4 -5 min H 2 . On the other hand, SEM observation of all spent samples revealed that Fe addition causes a massive accumulation of carbon nanotubes under the latter cyclic condition but little at the former. Thus several sets of comparative tests were specially designed and performed to get insight into the rule of Fe-catalyzed cyclic formation of carbon nanotubes in stabilizing the activity at the cyclic condition of 5 min CH 4 -20 min H 2 . The results further confirmed that at this condition cyclic formation of carbon nanotubes enhances cyclic evolution of H 2 and makes the H 2 concentration of the system higher, which is thermodynamically beneficial for suppression of formation of the activity-deactivating surface coke. Finally, it was further confirmed that at least a 20 min H 2 exposure is required to remove most of the carbon nanotubes and surface coke formed during a 5 min CH 4 exposure and make most of Fe nanoparticles reactivated and available again for catalytic carbon nanotubes formation with an enhanced H 2 evolution, i.e., with a controlled formation of the surface coke in the next CH 4 exposure.