Cobalt-Containing Oxide Catalysts Obtained by The Sol-Gel Method with Auto-Combustion in The Reaction of Low-Temperature Oxidation of Carbon Monoxide

S. Zulfugarova
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Abstract

The reaction of low-temperature oxidation of carbon monoxide is important in the context of air purification and reduction of automotive emissions. Along with the search for active catalytic systems for carbon monoxide oxidation, the development of new energy-saving methods of catalyst synthesis also seems important. Cobalt-iron, cobalt-manganese, cobalt-chromium, cobalt-copper binary and cobalt-manganese-iron, cobalt-copper-iron-containing triple oxide systems for low-temperature oxidation of carbon monoxide into carbon dioxide were synthesized by the sol-gel method with auto-combustion. The samples were analyzed by X-ray diffraction, IR spectral and derivatographic methods of analysis, their specific surface area was measured by the BET method, micro-photographs were taken on a scanning electron microscope. It was established that the resulting binary and ternary cobalt-containing oxide systems are multiphase systems containing ferrites, manganites, and oxides of cobalt, copper, manganese, and iron. The resulting catalysts are active in the low-temperature oxidation of carbon monoxide at 145-180 °C. The activation energy of the CO oxidation reaction on the analyzed oxide systems was revealed by the Arrhenius equation is placed in the range of 17-33 kJ/mol. In the systems, an intensifying effect of the influence of its components on the catalytic activity is observed in the oxide and spinel phases. The Co-Cr=2:1 system, which, along with chromite, also contains cobalt oxide, which is active at a much lower temperature – 145 °C than systems with a Co-Cr=1:1 and 1:2 ratios. A similar dependence was obtained in the Co-Fe=2:1 system, i.e. in a sample that, along with cobalt ferrite, also contains cobalt oxide. On this catalyst, 100% conversion of CO to CO2 occurs at a temperature of 200 °C, and a Co-Fe = 1:2 sample with a stoichiometric ratio of metals, in which the ferritization reaction completely occurs, as experiments have shown, is active only at temperatures above 300 °C. The intensifying effect of the influence of the components on its activity is also observed in three-component systems, in which the complete conversion of CO occurs at a temperature of 145-160 °C. The appearance of various structural defects during short-term combustion of the gel without additional heat treatment, which can potentially be considered as catalytically active centers, on the one hand, and the presence of oxide and spinel phases in the composition of catalysts, which exhibit a mutual reinforcing effect, on the other hand, is demonstrative advantage of this method for the synthesis of active catalysts for low-temperature oxidation of carbon monoxide to dioxide.
溶胶-凝胶法在一氧化碳低温氧化反应中自燃烧制备含钴氧化物催化剂
一氧化碳低温氧化反应在空气净化和减少汽车尾气排放方面具有重要意义。随着对一氧化碳氧化活性催化系统的研究,开发新的节能催化剂合成方法也显得很重要。采用自燃烧的溶胶-凝胶法制备了低温氧化一氧化碳成二氧化碳的钴铁、钴锰、钴铬、钴铜二元和钴锰铁、钴铜铁三元氧化物体系。采用x射线衍射、红外光谱和衍生分析法对样品进行了分析,采用BET法测量了样品的比表面积,并在扫描电子显微镜下拍摄了显微照片。确定了二元和三元含钴氧化物体系是含铁氧体、锰酸盐以及钴、铜、锰和铁的氧化物的多相体系。所制得的催化剂在145 ~ 180℃的一氧化碳低温氧化反应中具有活性。根据Arrhenius方程,所分析的氧化体系中CO氧化反应的活化能在17 ~ 33kj /mol之间。在该体系中,氧化相和尖晶石相的组分对催化活性的影响越来越大。Co-Cr=2:1的体系,与铬铁矿一起,还含有氧化钴,它在145°C的温度下具有活性,比Co-Cr=1:1和1:2的体系低得多。在Co-Fe=2:1体系中也获得了类似的依赖关系,即在样品中,除了钴铁氧体,还含有钴氧化物。在该催化剂上,CO在200℃的温度下100%转化为CO2,而CO - fe = 1:2的金属化学计量比样品中,铁化反应完全发生,实验表明,只有在300℃以上的温度下才有活性。在三组分体系中,CO的完全转化发生在145-160℃的温度下,组分对其活性的影响也在增强。在没有额外热处理的情况下,凝胶在短期燃烧过程中出现的各种结构缺陷,一方面可能被认为是催化活性中心,另一方面,催化剂组成中存在氧化物和尖晶石相,它们表现出相互增强的作用,这表明该方法在合成一氧化碳低温氧化成二氧化碳的活性催化剂方面具有优势。
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