Synergistic Effect of the Catalytic Action of Copper and Cerium in the Oxidation of Carbon Monoxide on Modified Cu/Ce/ZSM-5 Zeolites

IF 1.3 4区 化学 Q4 CHEMISTRY, PHYSICAL
I. A. Ivanin, T. V. Kruchinin, O. V. Udalova, M. A. Tedeeva, M. I. Shilina
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Abstract

A series of mono- and bimetallic copper–cerium catalysts based on ZSM-5 zeolite with different aluminum content (SiO2/Al2O3 = 30 and 55) was synthesized by incipient wetness impregnation. The copper content was 0–4.3 wt %, and cerium loading varied in a range from 0 to 6 wt %. The resulting composites were studied by low-temperature nitrogen adsorption–desorption, X-ray photoelectron spectroscopy (XPS), electron paramagnetic resonance (EPR) spectroscopy, UV–Vis diffuse reflectance spectroscopy, and diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy of adsorbed CO and tested in the catalytic reaction of CO oxidation with oxygen. A pronounced synergistic effect of catalytic action of copper and cerium associated with the redox interaction between the metals was observed in the systems under study. The catalytic activity of the composites monotonically increased with the fraction of cerium in the bimetallic systems (as the Сu : Ce ratio was changed from 6 to 1). In the presence of the most active catalysts, the temperature at which CO conversion reached 50% was about 100°C. A decrease in the aluminum content of the zeolite contributed to higher catalytic activity. It was found that Cu+ ions bound to the surface of CeO2 particles played a key role in catalysis.

Abstract Image

铜和铈在改性Cu/Ce/ZSM-5分子筛上催化氧化一氧化碳的协同作用
采用初湿浸渍法合成了一系列基于不同铝含量(SiO2/Al2O3=30和55)的ZSM-5沸石的单金属和双金属铜铈催化剂。铜含量为0–4.3 wt%,铈负载量在0至6 wt%范围内变化。通过低温氮吸附-脱附、X射线光电子能谱(XPS)、电子顺磁共振(EPR)光谱、紫外-可见漫反射光谱和吸附CO的漫反射红外傅立叶变换(DRIFT)光谱对所得复合材料进行了研究,并在CO与氧氧化的催化反应中进行了测试。在所研究的系统中观察到铜和铈的催化作用与金属之间的氧化还原相互作用相关的显著协同效应。复合材料的催化活性随着双金属体系中铈的含量而单调增加(当Сu:Ce的比例从6变为1时)。在最具活性的催化剂存在的情况下,CO转化率达到50%的温度约为100°C。沸石中铝含量的降低有助于提高催化活性。研究发现,结合在CeO2颗粒表面的Cu+离子在催化中起着关键作用。
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来源期刊
Kinetics and Catalysis
Kinetics and Catalysis 化学-物理化学
CiteScore
2.10
自引率
27.30%
发文量
64
审稿时长
6-12 weeks
期刊介绍: Kinetics and Catalysis Russian is a periodical that publishes theoretical and experimental works on homogeneous and heterogeneous kinetics and catalysis. Other topics include the mechanism and kinetics of noncatalytic processes in gaseous, liquid, and solid phases, quantum chemical calculations in kinetics and catalysis, methods of studying catalytic processes and catalysts, the chemistry of catalysts and adsorbent surfaces, the structure and physicochemical properties of catalysts, preparation and poisoning of catalysts, macrokinetics, and computer simulations in catalysis. The journal also publishes review articles on contemporary problems in kinetics and catalysis. The journal welcomes manuscripts from all countries in the English or Russian language.
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