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Mn 价态和晶格氧在 Mn 基 TiO2 催化剂上对 NH3 低温选择性催化还原 NO 的影响。

Effect of the Mn oxidation state and lattice oxygen in Mn-based TiO2 catalysts on the low-temperature selective catalytic reduction of NO by NH3.

机构信息

Department of Environmental Energy Systems Engineering, Kyonggi University, 94 San, Iui-dong, Youngtong-ku, Suwon-si, Gyeonggi-do 442-760, South Korea.

出版信息

J Air Waste Manag Assoc. 2012 Sep;62(9):1085-92. doi: 10.1080/10962247.2012.696532.

Abstract

UNLABELLED

TiO2-supported manganese oxide catalysts formed using different calcination temperatures were prepared by using the wet-impregnation method and were investigated for their activity in the low-temperature selective catalytic reduction (SCR) of NO by NH3 with respect to the Mn valence and lattice oxygen behavior. The surface and bulk properties of these catalysts were examined using Brunauer-Emmett-Teller (BET) surface area, X-ray diffraction (XRD), temperature-programmed reduction (TPR), and temperature-programmed desorption (TPD). Catalysts prepared using lower calcination temperatures, which contained Mn4+ displayed high SCR activity at low temperatures and possessed several acid sites and active oxygen. The TPD analysis determined that the Brönsted and Lewis acid sites in the Mn/TiO2 catalysts were important for the low-temperature SCR at 80-160 and 200-350 degrees C, respectively. In addition, the available lattice oxygen was important for attaining high NO to NO2 oxidation at low temperatures.

IMPLICATIONS

Recently, various Mn catalysts have been evaluated as SCR catalysts. However, there have been no studies on the relationship of adsorption and desorption properties and behavior of lattice oxygen according to the valence state for manganese oxides (MnO(x)). Therefore, in this study, the catalysts were prepared by the wet-impregnation method at different calcination temperatures in order to show the difference of manganese oxidation state. These catalysts were then characterized using various physicochemical techniques, including BET, XRD, TPR, and TPD, to understand the structure, oxidation state, redox properties, and adsorption and desorption properties of the Mn/TiO2 catalysts.

摘要

未标记

使用不同煅烧温度的 TiO2 负载氧化锰催化剂通过湿浸渍法制备,并研究了它们在 NH3 低温选择性催化还原(SCR)NO 中的活性与 Mn 价态和晶格氧行为的关系。使用比表面积(BET)、X 射线衍射(XRD)、程序升温还原(TPR)和程序升温脱附(TPD)等方法对这些催化剂的表面和体相性质进行了考察。采用较低煅烧温度制备的催化剂,含有 Mn4+,在低温下表现出较高的 SCR 活性,并且具有多个酸位和活性氧。TPD 分析表明,Mn/TiO2 催化剂中的 Brönsted 和 Lewis 酸位分别对 80-160 和 200-350°C 范围内的低温 SCR 很重要。此外,低温下获得高的 NO 到 NO2 氧化率需要可用的晶格氧。

意义

最近,已经评估了各种 Mn 催化剂作为 SCR 催化剂。然而,对于锰氧化物(MnO(x))的价态而言,关于吸附和解吸性质和晶格氧行为之间的关系,还没有研究。因此,在这项研究中,通过湿浸渍法在不同的煅烧温度下制备了催化剂,以显示出锰氧化态的差异。然后使用各种物理化学技术,包括 BET、XRD、TPR 和 TPD,对这些催化剂进行了表征,以了解 Mn/TiO2 催化剂的结构、氧化态、氧化还原性能以及吸附和解吸性能。

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