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Characterization of the H2/NOx reaction process over the La0.9Ce0.1Co0.9Pd0.1O3-BaO/Al2O3 catalyst
Yu Lyu1, Gang Lyu1, Xiangyu Dong1
1State Key Laboratory of Engines, Tianjin University, Tianjin 300072, China.
Abstract:
An excellent textual properties and performance La0.9Ce0.1Co0.9Pd0.1O3-BaO/Al2O3 catalyst was synthesized. The reaction mechanism of H2/NOx over the La0.9Ce0.1Co0.9Pd0.1O3-BaO/Al2O3 catalyst was investigated by temperature programmed reduction/ desorption/ surface reaction (TPR/D/SR) technologies and in-situ diffuse reflectance Fourier transform (DRIFT) technology. The results show that cerium or palladium species are inserted into the cells of LaCoO3, as well as they synergetic promote the redox properties of the La0.9Ce0.1Co0.9Pd0.1O3-BaO/Al2O3 catalyst. Surface activated nitrates exist over the La0.9Ce0.1Co0.9Pd0.1O3-BaO/Al2O3 catalyst, with thermal stable increasing in the order: absorbed N2O4 < monodentate nitrates < chelating bidentate nitrates < nitrates unidentate < free ionic nitrates < bulk free ionic nitrates. H2 preferentially reacted with absorbed N2O4 and monodentate nitrates at low temperatures, due to their high activity. The concentration of generated NH3 from the redox reaction of H2/NOx achieves the maximum value between 350 and 450 °C over the La0.9Ce0.1Co0.9Pd0.1O3-BaO/Al2O3 catalyst. Compared with the NOx adsorption process at 50 °C, monodentate nitrates and absorbed N2O4 disappeared due to their low thermal stability, chelating bidentate nitrates become stronger, as well as free ionic nitrates converted to bulk free ionic nitrates with higher thermal stability at 350 °C. When H2 is exposed to NOx species adsorbed on La0.9Ce0.1Co0.9Pd0.1O3-BaO/Al2O3, chelating bidentate nitrates and bulk free ionic nitrates are consumed gradually, indicating that although the bulk free ionic nitrates own high stability, it also could be consumed by involving in the H2/NOx reaction at 350 °C. The quantitative H2/NO reaction experiments confirmed the results of H2-TPSR and NSR. It is beneficial to the formation of NH3 when the H2/NO ratio is more than 2.5. Comparing traditional Pt-BaO/Al2O3 catalyst, the La0.9Ce0.1Co0.9Pd0.1O3-BaO/Al2O3 catalyst exhibit an excellent performance, including considerable NH3 production property, lower N2O selectivity, and the precious metal saving.
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