Chen Yajuan, Lou Diming, Zhang Yunhua, Fang Liang, Yang Dongxia
School of Automotive Studies, Tongji University, Shanghai 201804, China.
School of Automotive Studies, Tongji University, Shanghai 201804, China.
J Environ Sci (China). 2025 Sep;155:658-672. doi: 10.1016/j.jes.2025.01.018. Epub 2025 Jan 22.
The catalytic diesel particulate filter (CDPF) is the most widely used after-treatment device for controlling diesel engine soot emissions. The development of cost-effective catalysts is crucial for diesel engines to comply with future ultra-low emission regulations. This paper studies a new type of Ce/La modified Cs-V non-noble metal CDPF catalyst. Three test catalysts (Cs-V, Cs-V-5 %Ce, and Cs-V-5 %La) were formulated to explore the physical properties, activity, and sulfur resistance through XRD, SEM, XPS, and TPO tests. And TGA tests with different catalyst-to-soot mass ratios were designed to analyze the reaction kinetics. The results show that the soot oxidation process is divided into three stages: slow oxidation, rapid oxidation, and soot burnout. SEM and XRD results show that, compared with Ce doping, La-doped catalysts have less damage to the microstructure of the first active component, CsVO. XPS results show that the introduction of Ce and La is beneficial to the formation of oxygen vacancies and lattice distortion, increasing the proportion of active oxygen species, thereby improving the soot oxidation activity, among which La-doped active oxygen species have the highest proportion (94 %). And the Cs-V-5 %La catalyst has the best effect on improving the soot conversion of the three stages. The fresh state has the best low-temperature activity index, the lowest characteristic temperature (T of 374 °C) and activation energy (115.01 kJ/mol), and excellent sulfur resistance. The soot conversion and oxidation speed of the three stages decreases, duration lengthens, and activation energy increases by more than 100 kJ/mol as catalyst-to-soot mass ratios decrease.
催化型柴油颗粒过滤器(CDPF)是控制柴油发动机烟尘排放应用最为广泛的后处理装置。开发具有成本效益的催化剂对于柴油发动机符合未来超低排放法规至关重要。本文研究了一种新型的铈/镧改性的铯-钒非贵金属CDPF催化剂。制备了三种测试催化剂(铯-钒、铯-钒-5%铈和铯-钒-5%镧),通过X射线衍射(XRD)、扫描电子显微镜(SEM)、X射线光电子能谱(XPS)和程序升温氧化(TPO)测试来探究其物理性质、活性和抗硫性。并设计了不同催化剂与烟尘质量比的热重分析(TGA)测试来分析反应动力学。结果表明,烟尘氧化过程分为三个阶段:缓慢氧化、快速氧化和烟尘燃尽。扫描电子显微镜和X射线衍射结果表明,与铈掺杂相比,镧掺杂的催化剂对第一活性组分CsVO的微观结构破坏较小。X射线光电子能谱结果表明,铈和镧的引入有利于氧空位的形成和晶格畸变,增加了活性氧物种的比例,从而提高了烟尘氧化活性,其中镧掺杂的活性氧物种比例最高(94%)。铯-钒-5%镧催化剂对提高三个阶段的烟尘转化率效果最佳。新鲜状态下具有最佳的低温活性指标、最低的特征温度(374℃)和活化能(115.01kJ/mol)以及优异的抗硫性。随着催化剂与烟尘质量比降低,三个阶段的烟尘转化率和氧化速度降低,持续时间延长,活化能增加超过100kJ/mol。