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The dynamic behaviour of CH_3OH and NO_2 adsorbed on CeO_2 (111) studied by noncontact atomic force microscopy

机译:非接触原子力显微镜研究CH_3OH和NO_2吸附在CeO_2(111)上的动力学行为

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摘要

The adsorption and reaction of methanol (CH_3OH) and nitrogen dioxide (NO_2) on CeO_2(111) surfaces in different oxidation states were studied by noncontact atomic force microscopy (NC-AFM). After CH_3OH exposure, surface oxygen defects without reconstruction of the surrounding oxygen atoms were healed by methoxy species (CH_3O). Under a CH_3OH atmosphere, a heterogeneous feature in the reactivity of surface oxygen atoms to CH_3OH was observed by successive NC-AFM observation: new line defects of oxygen were produced as a result of a chemical event. Successive NC-AFM measurements also revealed that oxygen vacancies on a slightly reduced CeO_2 (111) surface were healed by exposure to NO_2. The contrast of healed oxygen defects in NC-AFM images was similar to that of other surface oxygen atoms. This indicates that dissociative adsorption of NO_2 occurred at the defects. Nitrogen trioxide (NO_3) was also observed on a slightly reduced CeO_2(111) surface after NO_2 exposure. On a CeO_2(111) surface without surface oxygen defects, neither adsorption of NO_2 nor formation of NO_3 was observed. The reaction mechanisms for the formation of line defects and NO_3 are discussed briefly.
机译:采用非接触原子力显微镜(NC-AFM)研究了甲醇(CH_3OH)和二氧化氮(NO_2)在CeO_2(111)表面上在不同氧化态下的吸附和反应。暴露于CH_3OH后,表面氧基缺陷(未重建周围的氧原子)被甲氧基物质(CH_3O)修复。在CH_3OH气氛下,通过连续的NC-AFM观察到了表面氧原子与CH_3OH的反应性的异质性特征:由于化学事件而产生了新的氧线缺陷。连续的NC-AFM测量还显示,通过暴露于NO_2,CeO_2(111)略微减少的表面上的氧空位已得到治愈。 NC-AFM图像中已修复氧缺陷的对比度与其他表面氧原子相似。这表明在缺陷处发生了NO_2的解离吸附。暴露NO_2后,在稍微还原的CeO_2(111)表面上也观察到三氧化二氮(NO_3)。在没有表面氧缺陷的CeO_2(111)表面上,未观察到NO_2的吸附或NO_3的形成。简要讨论了形成线缺陷和NO_3的反应机理。

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