Hydrothermal aging mechanism of K/CeO2 catalyst in soot catalytic combustion based on the Ostwald ripening mechanism

催化作用 热液循环 材料科学 奥斯特瓦尔德成熟 热重分析 化学工程 催化燃烧 烟灰 活化能 化学 燃烧 物理化学 纳米技术 有机化学 工程类
作者
Zonglin Li,Pan Wang,Chengcheng Ao,Zhongwei Meng,Lidong Zhang
出处
期刊:Thermal science and engineering progress [Elsevier]
卷期号:37: 101593-101593 被引量:4
标识
DOI:10.1016/j.tsep.2022.101593
摘要

The thermogravimetric analysis (TGA) experiment of CeO2 and K/CeO2 catalysts prepared with the incipient wetness impregnation method was carried out for the soot catalytic combustion at different K loadings before and after hydrothermal aging. The structure, morphology, and catalytic activity of CeO2 and K/CeO2 catalysts were thoroughly investigated with the means of N2 adsorption/desorption, XRD, XPS, and H2-TPR. The density functional theory (DFT) operation was applied to explain the mechanism of the decrease in catalytic activity of CeO2 and K/CeO2 catalysts after hydrothermal aging. TGA showed that the Tmax of the hydrothermal aging K/CeO2 catalyst was 505 °C, which was higher than CeO2 at 473 °C. After hydrothermal aging, CeO2 catalysts were less agglomerated than K/CeO2, and the ratio of Ce3+/Ce4+ decreases, but the mobile oxygen OII/OI ratio in the lattice were increased compared to CeO2 catalysts. DFT calculations showed that K doping significantly increases the surface energy and decreases the oxygen vacancy formation energy of (1 1 1), (2 0 0), (2 2 0), and (3 1 1) crystal planes, leading to enhanced catalytic combustion performance of the K/CeO2 catalyst soot based on the Mars-Van Krevelen mechanism. Furthermore, K doping decreased the adsorption energy of H2O and the energy barrier of K atoms diffusing near the surface of K/CeO2 catalyst crystals from 5.92 eV to 2.46 eV, which resulted in the loss of the active center number because of migration and coalescence (sintering) caused by crystal plane instability based on the Ostwald ripening mechanism.
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