Zeolitic-imidazolate framework precursors
(ZIF-67) were synthesized
in an inorganic solution with triethylamine as a deprotonating agent
for N2O decomposition, and the catalytic activities of
the pyrolysis products under different conditions were investigated.
Among them, the Co/CoO
x
@carbon catalyst
pyrolyzed at 650 °C in a N2 atmosphere (Co-650N) exhibited
excellent low-temperature catalytic activity and stability, achieving
50% decomposition efficiency at 305 °C and ∼100% at 400
°C, which benefitted from its large specific surface area, great
reduction performance, abundant cobalt active sites, and surface oxygen
species. Further, utilizing temperature-programmed desorption (TPD)
and in situ diffused reflectance infrared Fourier
transform spectroscopy (DRIFTS) results, it was found that N2O molecules preferentially combined with oxygen species bound to
cobalt sites. The absorbed N2O was decomposed into N2 and oxygen species, and the latter was subsequently transferred
to carbon frameworks. Interestingly, the amorphous graphitic carbon
frameworks played an important role in transferring/storing active
oxygen and regenerating cobalt sites. Moreover, Co-650N exhibited
better resistance to SO2, and the efficiency could be recovered
via heating and finally stabilized at 100%. Finally, the mechanisms
of N2O decomposition and sulfur poisoning-reactivation
on Co/CoO
x
@carbon catalysts were proposed
for the first time.