Ni2+改性铝酸铈的合成及其甲烷干重整制合成气反应的理化和催化性能研究

IF 1.2 4区 化学 Q4 CHEMISTRY, INORGANIC & NUCLEAR
A. A. Shutilov, A. S. Marchuk, G. A. Zenkovets
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引用次数: 0

摘要

采用溶液燃烧合成法制备了NixCe1-xAlO3 -δ催化剂(x = 0-0.5)。粉末XRD数据表明,产品在空气中700℃热处理主要形成铝酸铈相和少量高度分散的二氧化铈相。样品中镍含量的增加显著降低了二氧化铈相的含量。制备的Ni2+改性铝酸铈样品具有高比表面积和发达的多孔结构,是甲烷干重整反应(DRM)催化剂的前驱体。通过对这些样品在含氢气体混合物中进行初步还原(“活化”)后的物相组成和随后在反应介质条件下的性能研究表明,Ni2+离子被还原,从结构中出来到表面,形成尺寸为5-8 nm的金属Ni颗粒。研究了DRM反应中催化剂的化学组成对其性能的影响。具有代表性的Ni0.5Ce0.5AlO3 -δ催化剂在T = 700℃条件下反应30 h表现稳定,CH4转化率为77%,H2产率为43%,接触时间极短,τ为30 ms。所获得的催化剂在DRM反应中具有较高的催化活性是由于在Ni2+修饰的铝酸铈固有的大比表面积上形成了以高度分散的抗结焦金属Ni纳米颗粒为代表的活性相。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Synthesis of Ni2+-Modified Cerium Aluminate and Study of its Physicochemical and Catalytic Properties in the Dry Reforming of Methane Into Synthesis Gas Reaction

Synthesis of Ni2+-Modified Cerium Aluminate and Study of its Physicochemical and Catalytic Properties in the Dry Reforming of Methane Into Synthesis Gas Reaction

NixCe1–xAlO3–δ catalysts (x = 0-0.5) are prepared by the solution combustion synthesis method. According to the powder XRD data, thermal treatment of the products at 700 °C in air leads mainly to the formation of the cerium aluminate phase and to small amounts of highly dispersed cerium dioxide phase. An increase in the nickel content in the sample significantly decreases the content of the cerium dioxide phase. The prepared Ni2+-modified cerium aluminate samples are precursors of catalysts for the dry reforming of methane reaction (DRM) and are characterized by high specific surface area and a developed porous structure. The study of the phase composition of these samples after their preliminary reduction (“activation”) in a hydrogen-containing gas mixture and subsequent performance in the reaction medium conditions shows that the Ni2+ ions are reduced, come out from the structure to the surface, and form metal Ni particles with a size of 5-8 nm. The influence of catalysts′ chemical composition on their properties in the DRM reaction is studied. The representative Ni0.5Ce0.5AlO3–δ catalyst shows stable performance in the DRM reaction for 30 h at T = 700 °C with a CH4 conversion of 77%, an H2 yield of 43%, and an extremely short contact time τ of 30 ms. High catalytic activity of the obtained catalysts in the DRM reaction is due to the formation of the active phase represented by highly-dispersed coking-resistant metal Ni nanoparticles on the inherently large specific surface area of the Ni2+-modified cerium aluminate.

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来源期刊
Journal of Structural Chemistry
Journal of Structural Chemistry 化学-无机化学与核化学
CiteScore
1.60
自引率
12.50%
发文量
142
审稿时长
8.3 months
期刊介绍: Journal is an interdisciplinary publication covering all aspects of structural chemistry, including the theory of molecular structure and chemical bond; the use of physical methods to study the electronic and spatial structure of chemical species; structural features of liquids, solutions, surfaces, supramolecular systems, nano- and solid materials; and the crystal structure of solids.
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