二氧化碳合成高级碳氢化合物催化剂的研制

A. Trypolskyi
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摘要

本文致力于开发一种由二氧化碳和氢气合成高级碳氢化合物的催化剂。将温室气体二氧化碳转化为增值化学品不仅有助于解决环境问题,而且有助于获得有价值的燃料。在CO加氢反应中有活性的催化剂,在CO2加氢过程中也有活性。在二氧化碳的加氢反应中,最活跃的催化剂是基于过渡金属的,在过渡金属的存在下,主要形成甲烷和少量的一氧化碳。研究了过渡金属存在下二氧化碳加氢合成碳氢化合物的动力学,建立了该过程的机理,并没有对通过中间形成一氧化碳合成碳氢化合物的这种催化系统进行展望。确定了合成高级碳氢化合物的最佳方法是间接途径,即通过甲醇的中间生成并进一步脱水。在工业催化剂的存在下,由不同组分的H2、CO和CO2混合气体合成甲醇的宏观路线相同,即通过还原CO2,并伴有逆向水气转换反应。因此,不同成分的气体混合物可作为甲醇生产的原料。根据我们自己的数据和文献数据,得到了二氧化碳加氢反应的一般特性,从而可以开发出一种复杂的多功能催化剂,用于二氧化碳和氢气合成高级碳氢化合物。所提出的催化剂结合了从二氧化碳合成含氧化合物的催化剂和从乙醇和其他醇合成碳氢化合物的催化剂的特性。在研制的双功能催化剂上进行了支链烃含量较高的高烃的合成,并确定了最佳工艺条件。
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Development of catalysts for the synthesis of higher hydrocarbons from carbon dioxide
The paper is devoted to the development of a catalyst for the synthesis of the higher hydrocarbons from carbon dioxide and hydrogen. The conversion of greenhouse gas CO2 into value-added chemicals contributes not only to sol-ving environmental problems, but also to obtaining valuable fuel. Catalysts that are active in the hydrogenation reaction of CO are also active in the process of CO2 hydrogenation. The most active catalysts in the hydrogenation of carbon dioxide are based on transition metals, in the presence of which mainly methane and a small amount of carbon monoxide are formed. Investigation of the kinetics of hydrocarbons synthesis by hydrogenation of carbon dioxide in the presence of transition metals allowed establishing the mechanism of the process and no perspective of such catalytic systems for hydrocarbons synthesis via intermediate formation of carbon monoxide. It is established that the optimal method of synthesis of higher hydrocarbons is the indirect path, through the intermediate formation of methanol with its further dehydration. The synthesis of methanol from gas mixtures of H2, CO, and CO2 with different composition in the presence of industrial catalysts takes place along the same macroscopic route, by reducing CO2, and is accompanied by a reverse water-gas shift reaction. Therefore, gas mixtures of different composition can be used as raw material for methanol production. Based on our own and literature data, the general peculiarities of the carbon dioxide hydrogenation reaction were obtained, which allowed developing a complex multifunctional catalyst for the synthesis of higher hydrocarbons from carbon dioxide and hydrogen. The proposed catalyst combines the properties of ones for the synthesis of oxygenates from carbon dioxide, and catalysts for the processes of hydrocarbons synthesis from me-thanol and other alcohols. The synthesis of higher hydrocarbons with a predominant content of branched hydrocarbons on the developed bifunctional catalyst was carried out and the optimal conditions for the process were determined.
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