In this work, we investigated the mechanisms for the high activity and durability of Rh single nanosized catalysts for the CO–NO reaction in three-way catalysis. For this, we analyzed the relationship between the Rh particle morphology and surface adsorption of CO and NO molecules on Rh via transmission electron microscopy, in situ Fourier transform infrared (FT-IR) spectroscopy, and density functional theory calculations. Compared with that of the Rh-loaded catalyst as a conventional catalyst, we clearly found differences in the size of the Rh nanoparticles supported on the oxides. Additionally, one and two peaks were observed for CO adsorption on the Rh-loaded and Rh single nanosized catalysts via in situ FT-IR measurements, respectively, while the vibrational frequency of NO remained almost the same. The gemi-dicarbonyl CO adsorption, which corresponded to the two CO adsorption peaks in the Rh single nanosized catalyst, was only stable for small Rh nanoparticles, such as Rh₄. This indicated that the Rh particle size varied markedly between the Rh single nanosized and Rh-loaded catalysts. The adsorption properties of CO were different because of the particle size difference. We clearly found that the high catalytic activity of the Rh single nanosized catalyst was due to the small particle size of the supported Rh.

中文翻译：

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Rh基单纳米催化剂对CO和NO吸附性能的实验和计算研究

在这项工作中，我们研究了Rh单纳米催化剂在三效催化中CO-NO反应的高活性和耐久性的机理。为此，我们通过透射电子显微镜，原位傅立叶变换红外（FT-IR）光谱和密度泛函理论计算，分析了Rh颗粒形态与Rh上CO和NO分子在Rh上的表面吸附之间的关系。与作为常规催化剂的负载Rh的催化剂相比，我们清楚地发现了负载在氧化物上的Rh纳米颗粒的尺寸差异。另外，分别通过原位FT-IR测量观察到CO吸附在Rh负载和Rh单纳米催化剂上的一个和两个峰，而NO的振动频率几乎保持不变。双二羰基CO的吸附，₄。这表明Rh颗粒尺寸在Rh单纳米尺寸催化剂和Rh负载催化剂之间显着变化。由于粒径的不同，CO的吸附特性也不同。我们清楚地发现Rh单纳米催化剂的高催化活性归因于负载Rh的小粒径。