Gil-Barbarin Amaya, Gutiérrez-Ortiz José Ignacio, López-Fonseca Rubén, de Rivas Beatriz
Chemical Technologies for Environmental Sustainability Group, Department of Chemical Engineering, Faculty of Science and Technology, University of the Basque Country UPV/EHU, Barrio Sarriena s/n, Leioa E-48940, Bizkaia, Spain.
Ind Eng Chem Res. 2024 Feb 13;63(7):3003-3017. doi: 10.1021/acs.iecr.3c04045. eCollection 2024 Feb 21.
In this work, Ru-promoted cobalt oxide catalysts with a nanotube morphology were prepared by a synthesis route based on the Kirkendall effect followed by an acid treatment and subsequent optimized Ru impregnation. The resulting samples were thoroughly characterized by means of N physisorption, X-ray energy-dispersive spectroscopy, X-ray diffraction, scanning electron microscopy techniques, X-ray photoelectron spectroscopy, and temperature-programmed techniques (O-temperature-programmed desorption, H-temperature-programmed reduction, and temperature-programmed oxidation) and evaluated in the gas-phase oxidation of 1,2-dichloroethane. It has been demonstrated that Ru addition improves the oxygen mobility as well as the amount of Co and O species at the surface by the formation of the Ru-O-Co bond, which in turn governs the performance of the catalysts in the oxidation reaction. Moreover, the acid-etching favors the dispersion of the Ru species on the surface of the catalysts and strengthens the interaction among the noble metal and the cobalt oxide, thereby improving the thermal stability of the Ru-promoted oxides. Thus, the resulting catalysts are not only active, as the chlorinated pollutant is efficiently converted into deep oxidation products at relatively low temperatures, but also quite stable when operating for 120 h.
在本工作中，通过基于柯肯达尔效应的合成路线，随后进行酸处理和后续优化的Ru浸渍，制备了具有纳米管形态的Ru促进的氧化钴催化剂。通过N物理吸附、X射线能量色散光谱、X射线衍射、扫描电子显微镜技术、X射线光电子能谱和程序升温技术（O程序升温脱附、H程序升温还原和程序升温氧化）对所得样品进行了全面表征，并在1,2 - 二氯乙烷的气相氧化中进行了评估。结果表明，Ru的添加通过形成Ru - O - Co键提高了氧迁移率以及表面Co和O物种的数量，这反过来又决定了催化剂在氧化反应中的性能。此外，酸蚀刻有利于Ru物种在催化剂表面的分散，并加强了贵金属与氧化钴之间的相互作用，从而提高了Ru促进的氧化物的热稳定性。因此，所得催化剂不仅具有活性，因为氯化污染物在相对较低的温度下能有效地转化为深度氧化产物，而且在运行120小时时也相当稳定。
