Liaoning Key Laboratory of Clean Energy and Institute of Clean Energy and Environmental Engineering, College of Energy and Environment, Shenyang Aerospace University, 110034, Liaoning, People's Republic of China.
Beijing Key Laboratory for Solid Waste Utilization and Management, College of Engineering, Peking University, Beijing, 100871, People's Republic of China.
Environ Sci Pollut Res Int. 2017 Nov;24(31):24473-24484. doi: 10.1007/s11356-017-0084-1. Epub 2017 Sep 12.
A composite catalyst for the selective catalytic reduction (SCR) of NO with NH is investigated, in which the rare earth (RE, including La, Ce, Pr, and Nd) is doped into manganese oxides supported on activated semi-coke (MnO/ASC) via hydrothermal method at the molar ratio of Mn:RE = 1:5. It is evidenced that the addition of RE at a rather low molar ratio can enhance the catalytic activity of MnO/ASC. The catalyst with a Mn:Ce molar ratio of 10:1 yields an over 90% NO removal efficiency in the temperature range of 150-250 °C. An approximate 100% NO conversion and 95% N selectivity are achieved at about 200 °C. The catalysts are characterized by N physisorption, X-ray powder diffraction (XRD), scanning electron microscope (SEM), hydrogen temperature-programmed reduction (H-TPR) and X-ray photoelectron spectroscopy (XPS). The results indicated that the Ce additive is conducive to the NO adsorption and then accelerates the SCR reaction due to the formation of more chemisorbed oxygen (O), which is favored during the oxidation of NH and NO. Moreover, the in situ diffused reflectance infrared Fourier transform spectroscopy (DRIFTS) results confirm that the Ce additive on MnO/ASC catalyst could provide more active Brønsted acid sites, which eventually contributes to the SCR reaction. The generation of ad-NH and nitrite species is proved to play the crucial role in the promotional effect of RE addition.
一种用于 NH 选择性催化还原(SCR)NO 的复合催化剂,通过水热法在 Mn:RE=1:5 的摩尔比下将稀土(包括 La、Ce、Pr 和 Nd)掺杂到负载在活性半焦(MnO/ASC)上的锰氧化物中。结果表明,以较低的摩尔比添加 RE 可以提高 MnO/ASC 的催化活性。在 150-250°C 的温度范围内,Mn:Ce 摩尔比为 10:1 的催化剂的 NO 去除效率超过 90%。在 200°C 左右,NO 转化率接近 100%,N 选择性达到 95%。催化剂通过 N 物理吸附、X 射线粉末衍射(XRD)、扫描电子显微镜(SEM)、氢气程序升温还原(H-TPR)和 X 射线光电子能谱(XPS)进行了表征。结果表明,Ce 添加剂有利于 NO 的吸附,然后通过形成更多的化学吸附氧(O)加速 SCR 反应,这有利于 NH 和 NO 的氧化。此外,原位漫反射红外傅里叶变换光谱(DRIFTS)结果证实,MnO/ASC 催化剂上的 Ce 添加剂可以提供更多的活性 Brønsted 酸位,最终有助于 SCR 反应。证明了 ad-NH 和亚硝酸盐物种的生成在 RE 添加的促进作用中起着关键作用。