Direct N₂O decomposition over La₂NiO₄-based perovskite-type oxides

Abstract

Direct decomposition of N₂O by perovskite-structure catalysts including La₂NiO₄, LaSrNiO₄, and La_0.7Ce_0.3SrNiO₄ 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 La_0.7Ce_0.3SrNiO₄ are 44 and 36%, respectively, at 400ºC. As the temperature was increased to 600ºC, N₂O decomposition efficiency achieved with LaSrNiO₄ and La_0.7Ce_0.3SrNiO₄ 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 La_0.7Ce_0.3SrNiO₄ are not significantly affected as space velocity is increased from 8,000 to 20,000 hr⁻¹, while La_0.7Ce_0.3SrNiO₄ 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 La_0.7Ce_0.3SrNiO₄ 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 La_0.7Ce_0.3SrNiO₄ 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 La_0.7Ce_0.3SrNiO₄ 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.

Additional information

Notes on contributors

Kuan Lun Pan

Kuan Lun Pan is a Ph.D. student and Moo Been Chang is a distinguished professor at the Graduate Institute of Environmental Engineering, National Central University, Chungli, Taiwan.

Sheng Jen Yu

Sheng Jen Yu and Shaw Yi Yan are researchers at the Industrial Technology Research Institute (ITRI), Hsinchu, Taiwan.

Shaw Yi Yan

Sheng Jen Yu and Shaw Yi Yan are researchers at the Industrial Technology Research Institute (ITRI), Hsinchu, Taiwan.

Moo Been Chang

Kuan Lun Pan is a Ph.D. student and Moo Been Chang is a distinguished professor at the Graduate Institute of Environmental Engineering, National Central University, Chungli, Taiwan.