Rq. Long et Rt. Yang, Catalytic performance and characterization of VO2+-exchanged titania-pillared clays for selective catalytic reduction of nitric oxide with ammonia, J CATALYSIS, 196(1), 2000, pp. 73-85
VO2+ ion-exchanged TiO2-pillared clays (VO-TiO2-PILC) were investigated for
selective catalytic reduction of nitric oxide by ammonia in the presence o
f oxygen. They were also characterized for surface area and pore size distr
ibution and by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (X
PS), electron spin resonance (ESR), and Fourier transform infrared (FTIR) s
pectroscopy. It was found that VO-TiO2-PILC catalysts were highly active fo
r the selective catalytic reduction (SCR) reaction. The maximum activity wa
s obtained with 2.1-3.5 wt% vanadium, which was close to or slightly higher
than the activity of the commercial V2O5 + WO3/TiO2 catalyst. The VO-TiO2-
PILC catalysts were also resistant to water vapor and sulfur dioxide at hig
h temperatures (>350 degreesC). XRD patterns of VO-TiO2-PILC were similar t
o that of TiO2-PILC, showing no peaks due to vanadium oxides, even when the
vanadium content reached 13.2 wt%. XPS and ESR spectra indicated that vana
dium was present mainly as the +5 valence form (probably as V2O5) on the fr
esh catalysts, but was partially reduced to the +4 form (VO2+) after being
heated at 300 degreesC in He. The FTIR spectra of the adsorbed NO + O-2 sug
gested that vanadium oxides were anchored directly on the titania pillars o
f the catalysts. NH3 molecules adsorbed on the Bronsted acid and Lewis acid
sites to form, respectively, NH4+ ions and coordinated NH3 species. These
NH3 adspecies were active in reaction with NO and NO + O-2. The Bronsted ac
idity increased with increasing vanadium content, which was consistent with
an increase in the SCR activity for low temperatures (e.g., 200 degreesC).
By comparison, the adsorption of NOx (x = 1, 2) on the catalysts was very
weak, especially under reaction conditions. The present results indicate th
at the reaction path for NO reduction by NH3 on VO-TiO2-PILC is similar to
that on V2O5/TiO2; i.e., N-2 originates mainly from the reaction between ga
seous or weakly adsorbed NO and NH3 adspecies. (C) 2000 Academic Press.