Nitrous
oxide (N2O) originating from the combustion
of fossil fuels causes serious environmental issues. The design and
construction of a catalyst with high performance for the removal of
N2O remains challenging. Herein, a series of alkaline-earth
metal-modified A0.5Co2.5O4 (A = Mg,
Ca, Sr, Ba) catalysts were initiated by a hydrothermal protocol, and
their catalytic activities for N2O decomposition were systematically
investigated by experimental and density functional theory calculation.
The results reveal that the doping of alkaline-earth metals significantly
affects the morphology, structure, active oxygen species, oxygen vacancy,
and redox property and thereafter the catalytic activity of A0.5Co2.5O4 for N2O catalytic
decomposition. The introduction of alkaline-earth metals (A = Ca,
Sr, Ba) considerably promoted the reduction of Co3+ to
Co2+, thereby improving the electron-donating ability and
oxygen vacancy number and thereafter weakening the Co–O bond.
As a result, the catalytic activity of N2O decomposition
distinctively enhanced. Among them, Ba0.5Co2.5O4 shows optimal N2O decomposition performance
by virtue of its outstanding active oxygen species and excellent redox
property. However, the doping of Mg suppresses the electron-donating
ability of Mg0.5Co2.5O4 and thereafter
the catalytic activity for N2O decomposition. Therefore,
this work may shine light on the understanding of N2O decomposition
over alkaline-earth metal-modified Co-based oxides.