The amorphous Ce-Ti mixed oxides were reported to be catalysts for selective catalytic reduction of NO(x) with NH(3), in which Ce and not Ti acts as their solvent in spite of the fact that Ce is low in content. The amorphous catalysts were characterized by X-ray powder diffraction (XRD) and transmission electron microscopy (TEM) equipped with selective area electron diffraction (SAED). The Ce-Ti amorphous oxide shows higher activity than its crystalline counterpart at lower temperatures. Moreover, the presence of small CeO(2) crystallites as for the impregnated sample is deleterious to activity. The Ce-O-Ti short-range order species with the interaction between Ce and Ti in atomic scale was confirmed for the first time to be the active site using temperature programmed reduction with H(2) (H(2)-TPR), in situ FTIR spectra of NO adsorption, X-ray photoelectron spectroscopy (XPS), and X-ray absorption fine-structure (XAFS). Lastly, the Ce-O-Ti structure was directly observed by field-emission TEM (FETEM).
The soot combustion with NO(x) and/or O(2) on potassium-supported Mg-Al hydrotalcite mixed oxides under tight contact condition was studied using temperature-programmed oxidation (TPO), isothermal reaction and in situ FTIR techniques. The presence of NO(x) in O(2) favors the soot combustion at lower temperatures (<300 °C). However, a little suppression was observed at higher temperatures (>300 °C), which was accompanied by a substantial NO(x) reduction. The ketene (C═C═O) and isocyanate (NCO(-)) species were determined as the reaction intermediates. In NO(x) + O(2), NO(2) directly interacts with the free carbon sites (C═C*) through two parallel reactions: (1) NO(2) + C═C* → C═C═O + NO; (2) NO(2) + C═C* → NCO(-) + CO(2). The two reactions can proceed easily, which accounts for the promotion effect of NO(x) on soot combustion at lower temperatures. The further oxidation of NCO(-) by NO(2) or O(2) is responsible for the simultaneous reduction of NO(x). However, the reactions between NO(2) and C═C* are limited by the amount of free carbon sites, which can be provided by the oxidation of soot by O(2) at higher temperatures. The interaction of NO(x) and catalyst results in the formation of nitrates and nitrites, which poisoned the active K sites.
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