A sonochemical method is employed to synthesize LaNiO3 perovskites as catalysts for methane decomposition to produce
clean
CO
x
-free hydrogen and structured carbon.
The catalytic activities of perovskites prepared under various sonochemical
conditions (different power densities and exposure times) are contrasted
with those of LaNiO3 prepared by a conventional sol–gel
method. The results show that a sonochemically prepared catalyst presents
a methane conversion of up to 60% after 16 h of reaction, while the
conventional sol–gel LaNiO3 catalyst deactivates
quickly, reaching 1% methane conversion after 30 min of reaction.
Structural characterization of the as-prepared materials indicates
that under certain sonochemical conditions (low-intensity sonication
for 8 h) it is possible to obtain NiO inclusions in the LaNiO3 perovskite structure, which are not present when employing
the conventional synthesis technique. Upon activation of these materials
under reducing conditions, it is found that the presence of the sonochemically
formed NiO inclusions facilitates exsolution of the reduced Ni species
to the surface of the catalyst particles, improving the catalyst activity
in methane decomposition. The sonochemically synthesized catalysts,
which exhibit coexistence of LaNiO3 phase and NiO inclusions,
also seem to exhibit autocatalytic properties as they steer the methane
decomposition reaction toward formation of non-encapsulating carbon
nanotubes, which not only enhance catalyst stability but also increase
the catalyst activity over long reaction times.