Structural and Catalytic Properties of Rh–CeO2/MWCNT Composite Catalysts

IF 1.2 4区 化学 Q4 CHEMISTRY, INORGANIC & NUCLEAR
L. S. Kibis, A. V. Zadesenets, T. Yu. Kardash, S. V. Korenev, O. A. Stonkus, E. M. Slavinskaya, O. Yu. Podyacheva, A. I. Boronin
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Abstract

Composite catalysts consisting of Rh–CeOx structures supported on the surface of multi-walled carbon nanotubes (MWCNTs) are studied. For supported active components (Rh, Ce) the rhodium content is maintained constant on the MWCNT surface and the cerium concentration is varied in the range Rhat/Ceat = 0.085-0.34. The obtained samples are investigated by a combination of structural (X-ray diffraction, transmission electron microscopy (TEM)), spectral (X-ray photoelectron spectroscopy (XPS)), and kinetic (temperature-programmed reaction with CO (TPR-CO) and CO+O2 (TPR-CO+O2)) techniques. Highly dispersed CeO2 and RhOx particles are found to form in all samples studied. When the Rhat/Ceat ratio is changed, structures are formed that exhibit the catalytic activity in the CO oxidation reaction for different temperature ranges. At low Rhat/Ceat ratios (< 0.17) the CO conversion is observed at temperatures above 100 °C. When the Rhat/Ceat ratio increases, centers exhibiting the catalytic activity at temperatures below 0 °C are formed in Rh–CeO2/MWCNT catalysts. HR-TEM and TPR-CO studies of composite catalysts with a high Rhat/Ceat ratio reveal that structures based on dispersed oxidized rhodium particles modified by Ce3+ ions can be active species.

Abstract Image

Rh-CeO2/MWCNT 复合催化剂的结构和催化特性
摘要 研究了由支撑在多壁碳纳米管 (MWCNT) 表面的 Rh-CeOx 结构组成的复合催化剂。对于支撑的活性成分(Rh、Ce),MWCNT 表面的铑含量保持不变,铈浓度在 Rhat/Ceat = 0.085-0.34 范围内变化。我们结合结构(X 射线衍射、透射电子显微镜 (TEM))、光谱(X 射线光电子能谱 (XPS))和动力学(与 CO 的温度编程反应 (TPR-CO) 和 CO+O2 (TPR-CO+O2))技术对获得的样品进行了研究。在研究的所有样品中都发现形成了高度分散的 CeO2 和 RhOx 颗粒。当改变 Rhat/Ceat 比率时,形成的结构在不同温度范围内的 CO 氧化反应中表现出催化活性。当 Rhat/Ceat 比值较低时(0.17),二氧化碳的转化温度高于 100 °C。当 Rhat/Ceat 比率增加时,Rh-CeO2/MWCNT 催化剂中会形成在 0 °C 以下温度条件下具有催化活性的中心。对高 Rhat/Ceat 比的复合催化剂进行的 HR-TEM 和 TPR-CO 研究表明,基于分散的氧化铑颗粒经 Ce3+ 离子修饰的结构可以成为活性物种。
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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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