用于移动NH3-SCR的热稳定负载型V-W-TiO2催化剂的研制与表征

Q1 Materials Science Catalysis Structure & Reactivity Pub Date : 2015-02-01 DOI:10.1179/2055075814Y.0000000005
A. Beale, I. Lezcano‐González, T. Maunula, R. Palgrave
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引用次数: 29

摘要

摘要钒基催化剂负载在钨钛氧化物混合物(V2O5/ WO3-TiO2)上,对重型移动应用中NOx的氨选择性催化还原(NH3-SCR)具有很高的活性。然而,它们也被认为对高温敏感,这导致钛矿TiO2载体的烧结和金红石的一阶相变在600℃的温度下。在这里,我们报告了我们尝试使用SiO2来稳定TiO2锐钛矿相,并将其催化活性与未稳定的V2O5/ WO3-TiO2催化剂在高达800°C的热老化后的催化活性进行比较。为了了解高温对组分形态和催化界面的影响,还进行了光谱(拉曼光谱、紫外-可见光谱、x射线吸收光谱)、散射和提供催化表面信息的技术(Brunauer-Emmet-Teller、NH3吸附)的详细表征。结果表明,不稳定的V2O5/WO3 - TiO2催化剂在600℃热老化后初始稳定,但在600℃以上加热时,由于锐钛矿烧结并相变为金红石型TiO2,并且最初高度分散的WO3和聚合的V2O5相分离为单斜的WO3和V2O3晶体,催化活性明显下降。在700°C以上老化后,4-5 wt-%的sio2稳定样品也观察到类似的行为,因此重要的是,与不稳定样品相比,抵消了约100°C。
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Development and characterization of thermally stable supported V–W–TiO2 catalysts for mobile NH3–SCR applications
Abstract Vanadium based catalysts supported on a mixture of tungsten and titanium oxide (V2O5/WO3–TiO2) are known to be highly active for ammonia selective catalytic reduction (NH3–SCR) of NOx species for heavy-duty mobile applications. However they are also known to be sensitive to high temperatures which leads to both sintering of the anatase TiO2 support and a first order phase transition to rutile at temperatures >600°C. Here we report our attempts to use SiO2 to stabilize the TiO2 anatase phase and to compare its catalytic activity with that of a non-stabilized V2O5/WO3–TiO2 catalyst after thermal aging up to 800°C. Detailed characterization using spectroscopic (Raman, UV–vis, X-ray absorption spectroscopy), scattering and techniques providing information on the catalytic surface (Brunauer–Emmet–Teller, NH3 adsorption) have also been performed in order to understand the impact of high temperatures on component speciation and the catalytic interface. Results show that non-stabilized V2O5/WO3–TiO2 catalysts are initially stable after thermal aging at 600°C but on heating above this temperature a marked drop in catalytic activity is observed as a result of sintering and phase transformation of Anatase into Rutile TiO2 and phase segregation of initially highly dispersed WO3 and polymeric V2O5 into monoclinic WO3 and V2O3 crystallites. Similar behavior was observed for the 4–5 wt-% of SiO2-stabilised sample after aging above 700°C, importantly therefore, offset by some ∼100°C in comparison to the unstabilised sample.
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Catalysis Structure & Reactivity
Catalysis Structure & Reactivity CHEMISTRY, PHYSICAL-
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