采用尿素均相沉淀法合成了CuCeZrOx(CCZ)三元复合氧化物催化剂。采用X射线衍射分析(XRD)、N2-吸脱附测试、X射线光电子能谱(XPS)、扫描透射电镜(STEM)、程序升温还原(脱附、氧化)等技术, 考察煅烧温度对催化剂的物化性质和催化碳烟燃烧活性的影响。结果表明: 350℃煅烧产物CCZ-350表现出最优的催化活性: 在空速为12000 mL/(gcatalyst·h), O2浓度为10vol%, NO浓度为500×10–6, 催化剂和碳烟以10︰1质量比松散接触条件下, 碳烟颗粒最大燃烧速率温度T50 = 407℃, 同时表现出极佳的抗水汽中毒和抗SO2中毒性能, 这与活性组分的高度分散以及催化剂表面大量高活性吸附氧物种的存在有关。此外, 催化剂材料具有疏松多孔的鸟巢状结构, 有利于催化剂和碳烟颗粒的充分接触。该催化剂在柴油车尾气排放温度范围内(150-400℃)还能完全催化氧化柴油车尾气中CO、C3H6和C3H8等其他污染物, 显示出优异的催化净化柴油车尾气的综合性能。
A series of ternary composite oxides CuCeZrOx calcined at different temperatures were prepared by a homogeneous precipitation method using urea as the precipitant. X-ray diffraction (XRD), N2 adsorption-desorption analysis, X-ray photoelectron spectroscopy (XPS), scanning transmission electron microscope (STEM), and temperature-programmed reduction (or desorption, oxidation) (TPR, TPD or TPO) measurements were utilized to investigate the influence of calcination temperatures on the physicochemical property and catalysis performance towards soot catalytic oxidation. The CCZ-350 (calcined at 350℃) sample exhibits the optimized catalysis performance: temperature at the maximum rate of soot oxidation (T50) = 407℃, under test conditions of space velocity = 12000 mL/(gcatalyst·h), c(O2) = 10vol%, c(NO) = 500×10-6, and mass ratio of (loosely contacted) catalyst/soot = 10/1. It is believed that theabundant high-reactive adsorbed oxygen species on CCZ-350 surface contribute much to its outstanding catalysis performance. Besides, CCZ-350 with a loose-packing and porous morphology favors its sufficient contact with soot, thus further benefiting the catatlytic activity towards soot combustion. More importantly, CCZ-350 also presents good water vapor and SO2 resistence performance as well as good capability of eliminating other pollutants in diesel exhaust at low temperatures (150-400℃), such as CO, C3H6 and C3H8.