Investigation on Fe-Co binary metal oxides supported on activated semi-coke for NO reduction by CO

吸附 化学 催化作用 物理吸附 氧化还原 X射线光电子能谱 焦炭 金属 无机化学 氮氧化物 热液循环 化学工程 比表面积 有机化学 燃烧 工程类
作者
Luyuan Wang,Xingxing Cheng,Zhiqiang Wang,Chunyuan Ma,Yukun Qin
出处
期刊:Applied Catalysis B-environmental [Elsevier BV]
卷期号:201: 636-651 被引量:223
标识
DOI:10.1016/j.apcatb.2016.08.021
摘要

In this study, different amounts of Fe and Co species were loaded on activated semi-coke (ASC) using a hydrothermal method for the reduction of NO by CO. The series of prepared catalysts were characterized by SEM, N2 physisorption, ICP, XRD, XPS, H2-TPR, and in situ DRIFTS, as well as ESR and Raman spectroscopy. In addition, the denitration (deNOx) performance and water/SO2 resistance were investigated. The precursor solution with a molar ratio of 0.8:0.2 for Fe:Co (Fe0.8Co0.2/ASC) produced spherical clusters that were uniformly dispersed on the surface. Moreover, Fe0.8Co0.2/ASC exhibited the most effective deNOx activity. The highest deNOx activity for Fe0.8Co0.2/ASC (determined from the characterization) was attributed to the high fraction of Brønsted acid sites, high possibility for the formation of oxygen vacancies, and a strong redox performance. The DRIFTS results suggested a possible mechanism involving the adsorption of NO on the Fe0.8Co0.2/ASC surface, followed by its transformation to nitrates or nitrite/nitro species. At low temperatures (<200 °C), nitrates were predominantly adsorbed on the surface and could react with CO species, affording CO2 and N2O. However, with increasing reaction temperatures (>200 °C), the coordinated nitrates and CO species on the surface reacted with the produced CO2 and N2. The effects of water and SO2 on the deNOx performance were examined. In the presence of only water, the deNOx performance decreased because of the competitive adsorption with NO, and in the presence of only SO2, reversible deactivation was observed; however, if both water and SO2 were present, irreversible catalyst deactivation was observed.
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