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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Reactions of Neutral Platinum Clusters with N_2O and CO
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Reactions of Neutral Platinum Clusters with N_2O and CO

机译：中性铂簇与N_2O和CO的反应

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摘要

The reduction of N_2O in the gas phase by isolated, neutral platinum clusters, Pt_(n = 4?12), was investigated using mass spectrometry. The associated oxygen transfer reactions had the general formula Pt_nO_(m?1) + N_2O → Pt_nO_m + N_2 (m = 1 or 2). The rate constants k1 and k2 for the reactions in which m = 1 and 2, respectively, were ascertained and were found to be similar to one another. Unexpectedly, Pt_6O was discovered to be completely unreactive with N_2O under the applied experimental conditions. The reaction mechanism was elucidated on the basis of density functional theory (DFT) calculations, which indicated a reaction barrier between Pt_6O + N_2O and Pt_6O_2 + N_2. The possibility of catalyzing either the reduction of N_2O or the oxidation of CO using neutral Ptn species was also examined and the results showed that Pt_n does not exhibit significant catalytic properties and that O and CO instead coadsorb to Pt_n. Desorption of CO_2 from the coadsorbed clusters was not clearly identifiable from mass spectra. The reactivities of the platinum clusters were discussed and compared with the properties of the highly catalytically active rhodium clusters.
机译：使用质谱研究了孤立的中性铂簇Pt_（n = 4？12）在气相中还原N_2O的情况。相关的氧转移反应具有通式Pt_nO_（m≥1）+ N_2O→Pt_nO_m + N_2（m ＝ 1或2）。确定了其中m = 1和2的反应的速率常数k1和k2，并且发现它们彼此相似。出乎意料的是，在所应用的实验条件下，发现Pt_6O与N_2O完全不反应。根据密度泛函理论（DFT）计算阐明了反应机理，表明了Pt_6O + N_2O与Pt_6O_2 + N_2之间的反应势垒。还研究了使用中性的Ptn物种催化N_2O还原或CO氧化的可能性，结果表明Pt_n没有显着的催化性能，而O和CO却共吸附到Pt_n上。从质谱图中不能清楚地识别出CO_2从共吸附簇中的解吸。讨论了铂簇的反应性，并将其与高催化活性铑簇的性质进行了比较。

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