催化作用
氧化物
吸附
氧化还原
X射线光电子能谱
拉曼光谱
高分辨率透射电子显微镜
催化氧化
晶体结构
氧气
无机化学
化学
材料科学
化学工程
结晶学
物理化学
纳米技术
生物化学
有机化学
透射电子显微镜
工程类
物理
光学
作者
Md Robayet Ahasan,Yifan Wang,Ruigang Wang
标识
DOI:10.1016/j.mcat.2021.112085
摘要
Gas adsorption-desorption processes on oxide supported metal catalysts are critical steps for understanding catalytic CO oxidation mechanism. This report investigates the support structure (shape and exposed crystal planes)-catalytic activity relationship of irreducible SiO2 and reducible CeO2 nanorods (NR) and nanocubes (NC) supported CuOx via various structural and surface characterization methods, including XRD, Raman spectroscopy, BET surface area, H2-TPR, CO-TPD, in situ DRIFTS, XPS, and HRTEM. Evidence is presented that both isolated Cu+/Cu2+ redox pair and lattice oxygen of oxide supports from different crystal planes (111, 011, and 001) of CeO2 play important role towards CO oxidation by supporting Langmuir–Hinshelwood mechanism. The Cu+/Cu2+ and Ce3+/Ce4+ species at CuOx-CeO2 interfaces can facilitate the charge and mass transfer between CuOx nanoclusters and CeO2 by electronic interaction which was highly promoted by reducible CeO2 NR support. In addition, CeO2 NR contains significantly higher amount of surface defects including oxygen vacancy, steps, voids, and lattice distortion on various crystal facets, which promote surface oxygen release of CeO2 and CO adsorption and oxidation on catalytically active sites at lower temperature. According to the CO oxidation results, the oxidized CuO/CeO2 NR sample showed 62.8% CO conversion at 100°C and up to 98.9% conversion at 397 °C.
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