In situ observation of highly oxidized Ru species in Ru/CeO2 catalyst under propane oxidation,Journal of Materials Chemistry A

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In situ observation of highly oxidized Ru species in Ru/CeO2 catalyst under propane oxidation
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2022-08-02 , DOI: 10.1039/d2ta02330j
Oleksii Bezkrovnyi ₁ , Mykhailo Vorokhta ₂ , Mirosława Pawlyta ₃ , Maciej Ptak ₁ , Lesia Piliai ₂ , Xianxian Xie ₂ , Thu Ngan Dinhová ₂ , Ivan Khalakhan ₂ , Iva Matolínová ₂ , Leszek Kepinski ₁

Affiliation

In this work, we prepared a promising catalyst for propane oxidation composed of ruthenium supported on polycrystalline hollow CeO₂ nanospheres. It was found that the Ru loading on the CeO₂ support strongly improves its catalytic activity, decreasing the T₅₀ by about 200 °C (from 500 to about 300 °C). By utilizing several ex situ techniques (XRD, HR-STEM, Raman spectroscopy, ICP analysis) and in situ NAP-XPS, we investigated the effect of different pre-treatments (calcination, reduction, and C₃H₈ oxidation reaction) on the morphology, structure, and chemical state of the Ru/CeO₂ catalyst. The correlations between the chemical state of ruthenium in the Ru/CeO₂ catalyst and its activity in C₃H₈ oxidation received particular attention. Here, it is shown for the first time that the Ru/CeO₂ interaction with an oxygen-rich atmosphere (C₃H₈ + O₂ (1 : 10)) at ≥300 °C results in ruthenium oxidation to volatile RuO₄, leading to Ru evaporation/desorption from the outer surface and homogeneous high dispersion inside the powder catalyst.

中文翻译：

丙烷氧化下Ru/CeO2催化剂中高度氧化的Ru物种的原位观察

在这项工作中，我们制备了一种有前景的丙烷氧化催化剂，该催化剂由负载在多晶空心 CeO ₂纳米球上的钌组成。发现负载在 CeO ₂载体上的 Ru 极大地提高了其催化活性，使T ₅₀降低了约 200 ℃（从 500 至约 300 ℃）。通过利用多种非原位技术（XRD、HR-STEM、拉曼光谱、ICP 分析）和原位NAP-XPS，我们研究了不同预处理（煅烧、还原和 C ₃ H ₈氧化反应）对Ru/CeO ₂的形貌、结构和化学状态催化剂。_{Ru/CeO 2}催化剂中钌的化学状态与其在C ₃ H ₈氧化中的活性之间的相关性受到特别关注。在这里，首次表明，在≥300 °C 时，Ru/CeO ₂与富氧气氛 (C ₃ H ₈ + O ₂ (1 : 10)) 的相互作用导致钌氧化为挥发性的 RuO ₄，导致Ru从外表面蒸发/解吸并在粉末催化剂内部均匀高分散。

更新日期：2022-08-02

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