Ag supported on CeO2 with different morphologies for the catalytic oxidation of HCHO

催化作用 X射线光电子能谱 氧气 空间速度 拉曼光谱 催化氧化 空位缺陷 纳米颗粒 纳米棒 化学 热液循环 化学工程 材料科学 无机化学 光化学 结晶学 纳米技术 选择性 有机化学 物理 光学 工程类
作者
Lian Yu,Ruosi Peng,Limin Chen,Mingli Fu,Junliang Wu,Daiqi Ye
出处
期刊:Chemical Engineering Journal [Elsevier]
卷期号:334: 2480-2487 被引量:121
标识
DOI:10.1016/j.cej.2017.11.121
摘要

Ag/CeO2 catalysts with various shapes of CeO2 (nanorods, nanoparticles, and nanocubes) were prepared by the hydrothermal and impregnation method and then used for the catalytic oxidation of HCHO at low temperature. TEM and XRD results showed that Ag nanoparticles were well dispersed on the surface of CeO2. According to the results from XPS, H2-TPR and Raman spectra, Ag/r-CeO2, Ag/p-CeO2 and Ag/c-CeO2 exhibited different oxygen vacancy concentration, more oxygen vacancy and surface chemisorbed oxygen formed in Ag/r-CeO2. There might existed synergetic interaction between Ag and CeO2, and the presence of Ag nanoparticles could promoted the activation of surface chemisorbed oxygen, which is favorable for HCHO oxidation. The catalytic properties of the catalysts were significantly dependent on the shapes of CeO2, due to the highest surface oxygen vacancy concentration and best reducibility, Ag/r-CeO2 exhibited the best catalytic activity for HCHO oxidation. Ag/r-CeO2 showed higher specific reaction rate (7.43 nmol/(s·m2) at 100 °C) and TOFAg (0.0071 s−1 at 100 °C) under 810 ppm of HCHO and 84,000 h−1 of GHSV. Ag/r-CeO2 could reach complete HCHO oxidation at around 110 °C, which was lower than that of Ag/p-CeO2 and Ag/c-CeO2. Higher low-temperature reducibility, more surface oxygen vacancies, surface lattice oxygen species, and lattice defects produced by the interaction of Ag and CeO2 contributed to the excellent catalytic performance of Ag/r-CeO2 for HCHO oxidation. These results revealed that the HCHO catalytic oxidation activity was dependent on the shapes of CeO2 supports, this study suggested that the catalytic activity of the metal/CeO2 catalysts can be regulated by engineering the shapes of CeO2 supports.
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