School of Environmental Science and Technology, Dalian University of Technology, Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education, China), Dalian 116024, China.
School of Environmental & Chemical Engineering, Dalian Jiaotong University, Dalian 116028, China.
J Hazard Mater. 2016 Jan 15;301:512-21. doi: 10.1016/j.jhazmat.2015.09.024. Epub 2015 Sep 15.
The development of catalysts for selective catalytic reduction (SCR) reactions that are highly active at low temperatures and show good resistance to SO2 and H2O is still a challenge. In this study, we have designed and developed a high-performance SCR catalyst based on nano-sized ceria encapsulated inside the pores of MIL-100(Fe) that combines excellent catalytic power with a metal organic framework architecture synthesized by the impregnation method (IM). Transmission electron microscopy (TEM) revealed the encapsulation of ceria in the cavities of MIL-100(Fe). The prepared IM-CeO2/MIL-100(Fe) catalyst shows improved catalytic activity both at low temperatures and throughout a wide temperature window. The temperature window for 90% NOx conversion ranges from 196 to 300°C. X-ray photoelectron spectroscopy (XPS) and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFT) analysis indicated that the nano-sized ceria encapsulated inside MIL-100(Fe) promotes the production of chemisorbed oxygen on the catalyst surface, which greatly enhances the formation of the NO2 species responsible for fast SCR reactions.
开发低温下高活性、对 SO2 和 H2O 具有良好抗性的选择性催化还原(SCR)反应催化剂仍然是一个挑战。在本研究中,我们设计并开发了一种基于纳米氧化铈封装在 MIL-100(Fe) 孔内的高性能 SCR 催化剂,该催化剂将优异的催化能力与浸渍法(IM)合成的金属有机骨架结构相结合。透射电子显微镜(TEM)显示氧化铈封装在 MIL-100(Fe) 的腔体内。所制备的 IM-CeO2/MIL-100(Fe)催化剂在低温和宽温度范围内均表现出改善的催化活性。90%NOx 转化率的温度窗口范围为 196 至 300°C。X 射线光电子能谱(XPS)和原位漫反射红外傅里叶变换光谱(DRIFT)分析表明,封装在 MIL-100(Fe) 内的纳米氧化铈促进了催化剂表面化学吸附氧的生成,这极大地促进了负责快速 SCR 反应的 NO2 物种的形成。