In this review we focus on the catalytic removal of a series of N-containing exhaust gases with various valences, including nitriles (HCN, CH3CN, and C2H3CN), ammonia (NH3), nitrous oxide (N2O), and nitric oxides (NO(x)), which can cause some serious environmental problems, such as acid rain, haze weather, global warming, and even death. The zeolite catalysts with high internal surface areas, uniform pore systems, considerable ion-exchange capabilities, and satisfactory thermal stabilities are herein addressed for the corresponding depollution processes. The sources and toxicities of these pollutants are introduced. The important physicochemical properties of zeolite catalysts, including shape selectivity, surface area, acidity, and redox ability, are described in detail. The catalytic combustion of nitriles and ammonia, the direct catalytic decomposition of N2O, and the selective catalytic reduction and direct catalytic decomposition of NO are systematically discussed, involving the catalytic behaviors as well as mechanism studies based on spectroscopic and kinetic approaches and molecular simulations. Finally, concluding remarks and perspectives are given. In the present work, emphasis is placed on the structure-performance relationship with an aim to design an ideal zeolite-based catalyst for the effective elimination of harmful N-containing compounds.
Transition metal (cerium and cobalt)
doped γ-MnO2 (M-γ-MnO2, where M
represents Ce, Co) catalysts
were successfully synthesized and characterized. Cerium-doped γ-MnO2 materials showed ozone (O3) conversion of 96%
for 40 ppm of O3 under relative humidity (RH) of 65% and
space velocity of 840 L g–1 h–1 after 6 h at room temperature, which is far superior to the performance
of the Co-γ-MnO2 (55%) and γ-MnO2 (38%) catalysts. Under space velocity of 840 L g–1 h–1, the conversion of ozone over the Ce-γ-MnO2 catalyst under RH = 65% and dry conditions within 96 h was
60% and 100%, respectively, indicating that it is a promising material
for ozone decomposition. XRD and HRTEM data suggested that Ce-γ-MnO2 formed mixed crystals consisting of α-MnO2 and γ-MnO2 with specific surface area increased
from 74 m2/g to 120 m2/g compared to undoped
γ-MnO2, thus more surface defects were introduced.
H2-TPR, O2-TPD, XPS, Raman, and EXAFS confirmed
that Ce-γ-MnO2 exhibited more surface oxygen vacancies
and surface defects, which play a key role during the decomposition
of ozone. This study provides important insights for developing improved
catalysts for gaseous ozone decomposition and promoting the performance
of manganese oxide for practical ozone elimination.
In this study, an economical way for SSZ-13 preparation with the essentially cheap choline chloride as template has been attempted. The as-synthesized SSZ-13 zeolite after ion exchange by copper nitrate solution exhibited a superior SCR performance (over 95% NOx conversion across a broad range from 150 to 400 °C) to the traditional zeolite-based catalysts of Cu-Beta and Cu-ZSM-5. Furthermore, the opportune size of pore opening (∼3.8 Å) made Cu-SSZ-13 exhibiting the best selectivity to N2 as well as satisfactory tolerance toward SO2 and C3H6 poisonings. The characterization (XRD, XPS, XRF, and H2-TPR) of samples confirmed that Cu-SSZ-13 possessed the most abundant Cu cations among three investigated Cu-zeolites; furthermore, either on the surface or in the bulk the ratio of Cu(+)/Cu(2+) ions for Cu-SSZ-13 is also the highest. New finding was announced that CHA-type topology is in favor of the formation of copper cations, especially generating much more Cu(+) ions than the others, rather than CuO. The activity test of Cu(CuCl)-ZSM-5 (prepared by a solid-state ion-exchange method) clearly indicated that Cu(+) ions could make a major contribution to the low-temperature deNOx activity. The activity of protonic zeolites (H-SSZ-13, H-Beta, H-ZSM-5) revealed the topology effect on SCR performances.
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