TiO2负载Mn-Co复合氧化物催化剂上NO催化氧化性能

氮氧化物(NO_x)是大气主要污染物之一, 主要来源于化石燃料的燃烧, 其中NO不溶于水难以去除, 催化氧化技术可以将NO氧化为易溶于水可被脱硫装置去除的NO₂, 具有十分重要的实际意义. 本文采用浸渍法制备了不同Mn掺杂量的Mn-Co/TiO₂复合金属氧化物催化剂, 考察了其催化NO氧化的活性. 结果表明, Mn的掺杂对Co/TiO₂催化剂催化NO氧化的活性有明显促进作用, 掺杂量为6%时, Mn(0.3)-Co(0.7)/TiO₂催化剂NO的转化效率最高, 300℃达到88%. 采用X射线衍射(XRD)、N₂吸附/脱附、H₂程序升温还原(H₂-TPR)、O₂程序升温脱附(O₂-TPD)和原位漫反射傅里叶变换红外(in-situ DRFTIR)光谱等技术对催化剂的物理化学特征进行了表征. 结果发现, 当掺杂量为6%时, Mn一方面促进了催化剂表面活性组分的分散, 增加了催化剂的比表面积和孔径; 另一方面提高了催化剂的还原性能, 促进氧的低温脱附, 此外还促进了反应中间产物桥式NO-3向NO₂的反应, 从而提高了Co/TiO₂催化剂的NO氧化活性.

Catalytic Oxidation Activity of NO on TiO2-Supported Mn-Co Composite Oxide Catalysts

Globally, NO_x is one of the most widespread pollutants. It is generated mainly from the burning of fossil fuels, and NO is very difficult to remove because of its capacity to be dissolved in water. The catalytic oxidation method can be used to convert NO to NO₂, which is soluble in water and can be removed using desulfurization devices. Here, a series of TiO₂-supported Mn-Co composite oxide catalysts were prepared using the impregnation method. The results of catalytic activity tests showed that the addition of Mn enhanced the efficiency of NO oxidation. Significantly, with 6% doping amounts, Mn (0.3)-Co(0.7)/TiO₂ showed the best activity of 88% NO conversion at 300 ° C. X-ray diffraction (XRD), N₂ adsorption/desorption, hydrogen temperature-programmed reduction (H₂-TPR), oxygen temperatureprogrammed desorption (O₂-TPD), and in-situ diffuse reflectance Fourier transform infrared (in-situ DRFTIR) spectroscopy were used to characterize the catalysts. The results indicated that when the doping amount was 6%, the Mn enhanced the specific surface areas and pore volumes, which improved the dispersion of the active component over the TiO₂ support. The co-doping of manganese into the Co/TiO₂ also enhanced the oxygen desorption capabilities of the catalysts, which improved their reduction abilities. In addition, bridge NO₃^-, the key intermediate, was converted into NO₂; this conversion was also enhanced by the presence of Mn on the Co/TiO₂ catalyst. All of the above reasons account for the high NO catalytic oxidation activity of the supported Mn-Co composite oxide catalysts.