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Phase composition, morphology, properties and improved catalytic activity of hydrothermally-derived manganese-doped ceria nanoparticles

机译:水热衍生锰掺杂氧化铈纳米颗粒的物相组成、形貌、性能及改进的催化活性

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Manganese-doped ceria nanoparticles were prepared by hydrothermal synthesis and the prepared samples were thermally treated at 500 degrees C for 2 h. The samples were investigated using x-ray diffraction (XRD), high-resolution transmission electron microscopy (HR-TEM), energy-dispersive x-ray spectroscopy (EDS), N-2 adsorption and x-ray photoelectron spectroscopy (XPS). XRD revealed that nanocrystalline ceria is the main phase in all samples, while a romanechite-like phase (Na2Mn5O10) appears in the sample doped with 30 of Mn. TEM coupled with EDS exposed the presence of the same phase in the sample doped with 20 Mn. While ceria particles have spherical morphology and particle size ranging from 4.3 to 9.2 nm, the rare crystals of the romanechite-like phase adopt a tubular morphology with a length of at least 1 mu m. However, the decrease in the ceria lattice constant and the EDS spectra of the ceria nanoparticles clearly indicate that a substantial amount of manganese entered the ceria crystal lattice. Manganese doping has a beneficial impact on the specific surface area of ceria. XPS measurements reveal a decrease in the Ce3+/Ce3+ + Ce4+ content in the doped samples which is replaced by Mn3+. Moreover, a drastic increase in adsorbed oxygen is observed in the doped samples which is the consequence of the increase in Mn3+ species that promotes oxygen migrations to the surface of the sample. Compared to the pure sample, the doped samples showed significantly higher catalytic activity for the process of toluene oxidation.
机译:采用水热合成法制备了锰掺杂的铈纳米颗粒,并在500°C下热处理了2 h。采用X射线衍射(XRD)、高分辨透射电子显微镜(HR-TEM)、能量色散X射线光谱(EDS)、N-2吸附和X射线光电子能谱(XPS)对样品进行了研究。XRD分析显示,纳米晶铈是所有样品中的主要相,而掺杂了30%Mn的样品中出现了类似罗曼内希石的相(Na2Mn5O10)。虽然铈颗粒具有球形形貌,粒径范围为4.3-9.2 nm,但稀有的罗曼内奇石相晶体采用长度至少为1 μ m的管状形态。然而,铈晶格常数的降低和铈纳米颗粒的EDS光谱清楚地表明,大量的锰进入了铈晶格。锰掺杂对铈的比表面积有有益的影响。XPS测量结果显示,掺杂样品中Ce3+/Ce3+++Ce4+含量降低,被Mn3+取代。此外,在掺杂样品中观察到吸附氧的急剧增加,这是 Mn3+ 物种增加的结果,这促进了氧向样品表面的迁移。与纯样品相比,掺杂样品对甲苯氧化过程的催化活性显著提高。

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