Sanchis Rut, Alonso-Domínguez Daniel, Dejoz Ana, Pico María Pilar, Álvarez-Serrano Inmaculada, García Tomás, López María Luisa, Solsona Benjamín
Departament d'Enginyeria Química, ETSE, Universitat de València, Av. Universitat, 46100 Burjassot, Valencia, Spain.
Departamento de Química Inorgánica, Facultad de Ciencias Químicas, Universidad Complutense de Madrid, 28040 Madrid, Spain.
Materials (Basel). 2018 Aug 9;11(8):1387. doi: 10.3390/ma11081387.
Iron oxides (FeOx) are non-toxic, non-expensive and environmentally friendly compounds, which makes them good candidates for many industrial applications, among them catalysis. In the present article five catalysts based on FeOx were synthesized by mild routes: hydrothermal in subcritical and supercritical conditions (Fe-HT, Few200, Few450) and solvothermal (Fe-ST1 and Fe-ST2). The catalytic activity of these catalysts was studied for the total oxidation of toluene using very demanding conditions with high space velocities and including water and CO₂ in the feed. The samples were characterized by X-ray diffraction (XRD), scanning and high-resolution transmission electron microscopy (SEM and HRTEM), X-ray photoelectron spectroscopy (XPS) and nitrogen adsorption-desorption isotherms. It was observed that the most active catalyst was a cavity-containing porous sample prepared by a solvothermal method with a relatively high surface area (55 m² g) and constituted by flower-like aggregates with open cavities at the catalyst surface. This catalyst displayed superior performance (100% of toluene conversion at 325 °C using highly demanding conditions) and this performance can be maintained for several catalytic cycles. Interestingly, the porous iron oxides present not only a higher catalytic activity than the non-porous but also a higher specific activity per surface area. The high activity of this catalyst has been related to the possible synergistic effect of compositional, structural and microstructural features emphasizing the role of the surface area, the crystalline phase present, and the properties of the surface.
氧化铁(FeOx)是无毒、廉价且环保的化合物,这使其成为许多工业应用(包括催化)的理想候选物。在本文中,通过温和的方法合成了五种基于FeOx的催化剂:亚临界和超临界条件下的水热法(Fe-HT、Few200、Few450)以及溶剂热法(Fe-ST1和Fe-ST2)。在非常苛刻的条件下,即高空速且进料中包含水和二氧化碳的情况下,研究了这些催化剂对甲苯完全氧化的催化活性。通过X射线衍射(XRD)、扫描和高分辨率透射电子显微镜(SEM和HRTEM)、X射线光电子能谱(XPS)以及氮气吸附-脱附等温线对样品进行了表征。观察到最具活性的催化剂是通过溶剂热法制备的含空腔的多孔样品,其具有相对较高的表面积(55 m² g),由催化剂表面带有开放空腔的花状聚集体构成。该催化剂表现出优异的性能(在325°C下使用苛刻条件时甲苯转化率达100%),并且这种性能可以在几个催化循环中保持。有趣的是,多孔氧化铁不仅比无孔的具有更高的催化活性,而且每单位表面积的比活性也更高。该催化剂的高活性与组成、结构和微观结构特征可能的协同效应有关,强调了表面积、存在的晶相以及表面性质的作用。