Nitrous oxide (N2O) is a potent greenhouse
gas with
a high global warming potential. The N2O direct decomposition
(deN2O) is currently the most widely used technique due
to its operational simplicity and lack of secondary pollution. The
presence of impurity gases in industrial exhaust increases the challenge
of eliminating N2O, urging the development of highly active
and stable catalysts for its degradation. In this study, a series
of praseodymium (Pr)-doped nickel oxide (NiO) catalysts were synthesized
for N2O degradation. These catalysts showed higher N2O decomposition activity (T
100 = 400–440 °C) than pure NiO (T
100 = 480 °C) and also demonstrated high resistance to
impurity gases in simulated industrial nitric acid tail gas. In the
catalyst with a Pr to Ni ratio of 0.002, the highly dispersed Pr on
the NiO surface regulated its particle size and increased specific
surface area and pore volume. DFT calculations revealed that Pr significantly
enhanced the electron-donating ability of Ni2+, facilitating
the dissociative adsorption of N2O on the catalyst surface,
where O existed in the form of Ni3+-O*. Additionally, Pr
reduced the desorption energy of O2, the rate-determining
step. During the reaction, Pr3+ transferred electrons to
Ni3+ via f-d electron hopping, stabilizing the active Ni2+ sites and enabling an efficient catalytic reaction. These
findings demonstrate the practical potential of this catalyst and
provide new insights into the degradation of N2O in industrial
exhaust gases, offering a promising avenue for application.