A series of novel metal-oxide-supported CeO(2) catalysts were prepared via the wet impregnation method, and their NH(3)-SCR activities were investigated. The Ce/TiO(2)-SiO(2) catalyst with a Ti/Si mass ratio of 3/1 exhibited superior NH(3)-SCR activity and high N(2) selectivity in the temperature range of 250-450 °C. The characterization results revealed that the activity enhancement was correlated with the properties of the support material. Cerium was highly dispersed on the TiO(2)-SiO(2) binary metal oxide support, and the interaction of Ti and Si resulted in greater conversion of Ce(4+) to Ce(3+) on the surface of the catalyst compared to that on the single metal oxide supports. As a result of in the increased number of acid sites on Ce/TiO(2)-SiO(2) that resulted from the addition of SiO(2), the NH(3) adsorption capacity was significantly improved. All of these factors played significant roles in the high SCR activity. More importantly, Ce/TiO(2)-SiO(2) exhibited strong resistance to SO(2) and H(2)O poisoning. After the addition of SiO(2), the number of Lewis-acid sites was not decreased, but the number of Brønsted-acid sites on the TiO(2)-SiO(2) carrier was increased. The introduction of SiO(2) further weakened the alkalinity over the surface of the Ce/TiO(2)-SiO(2) catalyst, which resulted in sulfate not easily accumulating on the surface of the Ce/TiO(2)-SiO(2) catalyst in comparison with Ce/TiO(2).
The structure determination of surface species has long been a challenge
because of their rich chemical heterogeneities. Modern tip-based microscopic
techniques can resolve heterogeneities from their distinct electronic, geometric,
and vibrational properties at the single-molecule level but with limited
interpretation from each. Here, we combined scanning tunneling microscopy (STM),
noncontact atomic force microscopy (AFM), and tip-enhanced Raman scattering (TERS)
to characterize an assumed inactive system, pentacene on the Ag(110) surface. This
enabled us to unambiguously correlate the structural and chemical heterogeneities
of three pentacene-derivative species through specific carbon-hydrogen bond
breaking. The joint STM-AFM-TERS strategy provides a comprehensive solution for
determining chemical structures that are widely present in surface catalysis,
on-surface synthesis, and two-dimensional materials.
Based on the ideas of the additives modification and regeneration method update, two different strategies were designed to deal with the traditional SCR catalyst poisoned by alkali metals. First, ceria doping on the V(2)O(5)-WO(3)/TiO(2) catalyst could promote the SCR performance even reducing the V loading, which resulted in the enhancement of the catalyst's alkali poisoning resistance. Then, a novel method, electrophoresis treatment, was employed to regenerate the alkali poisoned V(2)O(5)-WO(3)/TiO(2) catalyst. This novel technique could dramatically enhance the SCR activities of the alkali poisoned catalysts by removing approximately 95% K or Na ions from the catalyst and showed less hazardous to the environment. Finally, the deactivation mechanisms by the alkali metals were extensively studied by employing both the experimental and DFT theoretical approaches. Alkali atom mainly influences the active site V species rather than W oxides. The decrease of catalyst surface acidity might directly reduce the catalytic activity, while the reducibility of catalysts could be another important factor.
A series of cerium-tungsten oxide catalysts was prepared by the co-precipitation method and was evaluated for the selective catalytic reduction of NO x by ammonia (NH 3 -SCR) over a wide temperature range. These catalysts were characterized by BET, XRD, XPS and H 2 -TPR analyses. The experimental studies demonstrated that, among cerium-tungsten oxides, CeO 2 -WO 3 with a Ce/W molar ratio of 3/2 exhibited the best activity toward NH 3 -SCR reactions, N 2 selectivity and SO 2 durability over a broad temperature range of 175-500°C at a space velocity of 47,000 h -1 . The strong interaction between Ce and W could be the main factor leading to the high activity of the CeO 2 -WO 3 mixed oxide catalyst.
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