Abstract
Direct decomposition of N2O by perovskite-structure catalysts including La2NiO4, LaSrNiO4, and La0.7Ce0.3SrNiO4 was investigated. The catalysts were prepared by the Pechini method and characterized by x-ray diffraction (XRD), BET, scanning electron microscopy (SEM), and O2-TPD. Experimental results indicate that the properties of La2NiO4 are significantly improved by partially substituting La with Sr and Ce. N2O decomposition efficiencies achieved with LaSrNiO4 and La0.7Ce0.3SrNiO4 are 44 and 36%, respectively, at 400ºC. As the temperature was increased to 600ºC, N2O decomposition efficiency achieved with LaSrNiO4 and La0.7Ce0.3SrNiO4 reached 100% at an inlet N2O concentration of 1,000 ppm, while the space velocity was fixed at 8,000 hr−1. In addition, effects of various parameters including oxygen, water vapor, and space velocity were also explored. The results indicate that N2O decomposition efficiencies achieved with LaSrNiO4 and La0.7Ce0.3SrNiO4 are not significantly affected as space velocity is increased from 8,000 to 20,000 hr−1, while La0.7Ce0.3SrNiO4 shows better tolerance for O2 and H2O(g). On the other hand, N2 yield with LaSrNiO4 as catalyst can be significantly improved by doping Ce. At a gas hour space velocity of 8,000 hr−1, and a temperature of 600ºC, high N2O decomposition efficiency and N2 yield were maintained throughout the durability test of 60 hr, indicating the long-term stability of La0.7Ce0.3SrNiO4 for N2O decomposition.Implications:Nitrous oxide (N2O) not only has a high global warming potential (GWP100 = 310), but also potentially destroys ozone in the stratosphere. Pervoskite-type catalysts including La2NiO4, LaSrNiO4, and La0.7Ce0.3SrNiO4 are applied for direct N2O decomposition. The results show that N2O decomposition can be enhanced as Sr and Ce are doped into La2NiO4. At 600ºC, N2O decomposition efficiencies achieved with LaSrNiO4 and La0.7Ce0.3SrNiO4 reach 100%, demonstrating high activity and good potential for direct N2O decomposition. Effects of O2 and H2O(g) contents on catalytic activities are also evaluated and discussed.
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