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Rational design of 3D hierarchical foam-like Fe2O3@CuOx monolith catalysts for selective catalytic reduction of NO with NH3

机译:3D分层泡沫状Fe2O3 @ C​​uOx整体催化剂的合理设计,用于用NH3选择性催化还原NO

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Herein, we have rationally designed and originally fabricated a high-performance monolith catalyst based on 3D hierarchical foam-like Fe2O3@CuOx for selective catalytic reduction (SCR) of NO with NH3. The Fe2O3@CuOx foam catalyst was synthesized by calcining the Cu foam in air first to form CuOx foam with CuOx nanowire arrays on the surface and then the Fe2O3 could be in situ formed on the surface of CuOx through the reaction in the interfacial region between the aqueous solution of Fe2+ and CuO via a hydrothermal method. This catalyst was mainly characterized by the techniques of X-ray diffraction, transmission electron microscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, H-2 temperature-programmed reduction, NH3/NO + O-2 temperature-programmed desorption and in situ diffuse reflectance infrared Fourier transform spectroscopy. Both the atomic concentration of Cu+ and chemisorbed oxygen species are enhanced by the coating of Fe2O3, which facilitates NO attack on active sites, resulting in the in situ formation of NO2 and promoting the "fast SCR" reaction. Moreover, there is a strong interaction between CuOx and Fe2O3, which could not only lead to better reduction ability but also raise the acid amount and enhance the acid strength as well as NOx adsorption ability. Based on these favourable properties, the Fe2O3@CuOx catalyst exhibits a higher activity and more extensive operating temperature window than the catalyst without Fe2O3. More importantly, the Fe2O3 not only prevents the generation of ammonium sulfates from blocking the active sites but also inhibits the formation of copper sulfates, resulting in a high SO2-tolerance. In addition, the catalyst also displays favourable stability and H2O resistance. The rational design of 3D hierarchical foam-like Fe2O3@CuOx paves a new way for the development of environmentally-friendly and high-performance monolith deNO(x) catalysts.
机译:在这里,我们已经合理地设计和制造了一种基于3D分层泡沫状Fe2O3 @ C​​uOx的高性能整体式催化剂,用于用NH3选择性催化还原NO(SCR)。首先在空气中煅烧Cu泡沫形成表面带有CuOx纳米线阵列的CuOx泡沫合成Fe2O3 @ C​​uOx泡沫催化剂,然后通过两者之间的界面区的反应原位生成Fe2O3。通过水热法制备Fe2 +和CuO的水溶液。该催化剂的主要特点是通过X射线衍射,透射电子显微镜,扫描电子显微镜,X射线光电子能谱,H-2程序升温还原,NH3 / NO + O-2程序升温解吸和原位表征。漫反射红外傅里叶变换光谱。 Fe 2 O 3的涂层提高了Cu +和化学吸附氧物种的原子浓度,这促进了NO对活性位点的进攻,导致NO 2的原位形成并促进了“快速SCR”反应。而且,CuOx与Fe2O3之间存在很强的相互作用,这不仅可以导致更好的还原能力,而且可以增加酸量,增强酸强度以及NOx吸附能力。基于这些有利的性质,Fe2O3 @ C​​uOx催化剂比不含Fe2O3的催化剂具有更高的活性和更宽的工作温度范围。更重要的是,Fe2O3不仅防止硫酸铵的生成阻止活性位点,而且抑制了硫酸铜的形成,从而具有很高的SO2耐受性。另外,该催化剂还显示出有利的稳定性和耐H 2 O性。 3D分层泡沫状Fe2O3 @ C​​uOx的合理设计为开发环保高性能的整体式deNO(x)催化剂开辟了一条新途径。

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