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首页> 外文期刊>Chemistry: A European journal >Co-Adsorption of O-2 and CO on Au-2(-): Infrared Photodissociation Spectroscopy and Theoretical Study of [Au2O2(CO)(n)](-) (n=2-6)
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Co-Adsorption of O-2 and CO on Au-2(-): Infrared Photodissociation Spectroscopy and Theoretical Study of [Au2O2(CO)(n)](-) (n=2-6)

机译：O-2和CO在Au-2（-）上的共吸附：红外光解离光谱和[Au2O2（CO）（n）]（-）的理论研究（n = 2-6）

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摘要

The co-adsorption of O-2 and CO on anionic sites of gold species is considered as a crucial step in the catalytic CO oxidation on gold catalysts. In this regard, the [Au2O2(CO)(n)](-) (n=2-6) complexes were prepared by using a laser vaporization supersonic ion source and were studied by using infrared photodissociation spectroscopy in the gas phase. All the [Au2O2(CO)(n)](-) (n=2-6) complexes were characterized to have a core structure involving one CO and one O-2 molecule co-adsorbed on Au-2(-) with the other CO molecules physically tagged around. The CO stretching frequency of the [Au2O2(CO)](-) core ion is observed around (nu) over tilde =2032-2042cm(-1), which is about 200cm(-1) higher than that in [Au-2(CO)(2)](-).This frequency difference and the analyses based on density functional calculations provide direct evidence for the synergy effect of the chemically adsorbed O-2 and CO. The low lying structures with carbonate group were not observed experimentally because of high formation barriers. The structures and the stability (i.e., the inertness in a sense) of the co-adsorbed O-2 and CO on Au-2(-) may have relevance to the elementary reaction steps on real gold catalysts.
机译：O-2和CO在金的阴离子位点上的共吸附被认为是金催化剂上催化CO氧化的关键步骤。在这方面，[Au 2 O 2（CO）（n）]（-）（n ＝ 2-6）络合物是通过使用激光汽化超声离子源制备的，并且通过在气相中使用红外光解光谱学进行了研究。所有[Au2O2（CO）（n）]（-）（n = 2-6）配合物的特征是其核心结构包括一个CO和一个与Au-2（-）共吸附的O-2分子。其他CO分子在物理上被标记。在波浪号= 2032-2042cm（-1）周围（nu）处观察到[Au2O2（CO）]（-）核心离子的CO拉伸频率，比[Au-2]高200cm（-1）。 （CO）（2）]（-）。该频率差和基于密度泛函计算的分析为化学吸附的O-2和CO的协同效应提供了直接证据。实验未观察到具有碳酸酯基团的低洼结构因为形成障碍高。共吸附的O-2和CO在Au-2（-）上的结构和稳定性（从某种意义上说是惰性）可能与真实金催化剂上的基本反应步骤有关。

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