A novel
core–shell (ε-MnO2/CeO2)@CeO2 composite catalyst with a synergistic effect was
prepared by hydrothermal reaction and thermal decomposition and its
application to high-efficiency oxidation removal of formaldehyde (HCHO)
was systemically investigated. The (MnCO3/CeO2)@CeO2 precursor was prepared first by the one-pot hydrothermal
reaction of Mn2+ and Ce3+ solutions with a CO2-storage material (CO2SM) without any external
templates or surfactants required. The thermal decomposition of the
precursor afforded the core–shell (ε-MnO2/CeO2)@CeO2 composite catalyst with excellent catalytic
performance. HCHO in the feed gas (180 ppm HCHO, 21% O2, N2 balanced) at a gas hourly space velocity of 100 L/(gcat h) is 100% converted over the catalyst at 80 °C. The
conversion rate remains above 95% in 72 h and above 73.8% in 140 h,
suggesting the strong stability of the catalyst at high gas flow rates
and relatively low temperatures. The synergistic mechanism of the
catalyst was explored by X-ray diffraction, Raman, Brunauer–Emmett–Teller,
transmission electron microscopy, and X-ray photoelectron spectroscopy.
The number of defects in the catalyst and the strength of the Mn–O
bond in ε-MnO2 can be tuned by adjusting the synthesis
conditions. More oxygen vacancies on the surface of CeO2 can make the synergistic effect of the catalyst stronger, which
significantly improves the lattice oxygen (Olatt) activity
on the surface of ε-MnO2. Our work has provided new
insights into the preparation of the desired composite catalysts with
excellent performances.