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Catalytic Oxidation of NO over MnOx-CeO2 and MnOx-TiO2 Catalysts

机译:MnOx-CeO2和MnOx-TiO2催化剂上NO的催化氧化

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A series of MnOx-CeO2 and MnOx-TiO2 catalysts were prepared by a homogeneous precipitation method and their catalytic activities for the NO oxidation in the absence or presence of SO2 were evaluated. Results show that the optimal molar ratio of Mn/Ce and Mn/Ti are 0.7 and 0.5, respectively. The MnOx-CeO2 catalyst exhibits higher catalytic activity and better resistance to SO2 poisoning than the MnOx-TiO2 catalyst. On the basis of Brunauer-Emmett-Teller (BET), X-ray diffraction (XRD), and scanning transmission electron microscope with mapping (STEM-mapping) analyses, it is seen that the MnOx-CeO2 catalyst possesses higher BET surface area and better dispersion of MnOx over the catalyst than MnOx-TiO2 catalyst. X-ray photoelectron spectroscopy (XPS) measurements reveal that MnOx-CeO2 catalyst provides the abundance of Mn3+ and more surface adsorbed oxygen, and SO2 might be preferentially adsorbed to the surface of CeO2 to form sulfate species, which provides a protection of MnOx active sites from being poisoned. In contrast, MnOx active sites over the MnOx-TiO2 catalyst are easily and quickly sulfated, leading to rapid deactivation of the catalyst for NO oxidation. Furthermore, temperature programmed desorption with NO and O-2 (NO + O-2-TPD) and in situ diffuse reflectance infrared transform spectroscopy (in situ DRIFTS) characterizations results show that the MnOx-CeO2 catalyst displays much stronger ability to adsorb NOx than the MnOx-TiO2 catalyst, especially after SO2 poisoning.
机译:采用均相沉淀法制备了一系列MnOx-CeO2和MnOx-TiO2催化剂,并评估了它们在不存在或存在SO2的条件下对NO氧化的催化活性。结果表明,Mn / Ce和Mn / Ti的最佳摩尔比分别为0.7和0.5。 MnOx-CeO2催化剂比MnOx-TiO2催化剂具有更高的催化活性和更好的抗SO2中毒性。在Brunauer-Emmett-Teller(BET),X射线衍射(XRD)和具有标测的扫描透射电子显微镜(STEM映射)的基础上,可以看出MnOx-CeO2催化剂具有较高的BET表面积和MnOx在催化剂上的分散性优于MnOx-TiO2催化剂。 X射线光电子能谱(XPS)测量表明,MnOx-CeO2催化剂可提供大量的Mn3 +和更多的表面吸附氧,SO2可能优先吸附在CeO2的表面形成硫酸盐,从而保护了MnOx活性位从中毒。相反,在MnOx-TiO2催化剂上的MnOx活性位点容易快速硫酸化,导致NO氧化催化剂快速失活。此外,利用NO和O-2(NO + O-2-TPD)进行的程序升温解吸以及原位漫反射红外光谱(原位DRIFTS)表征结果表明,MnOx-CeO2催化剂显示出比NOx强得多的吸附能力。 MnOx-TiO2催化剂,尤其是在SO2中毒后。

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