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首页> 外文期刊>ACS catalysis >Carbon Number Dependence of Reaction Mechanism and Kinetics in CO Hydrogenation on a Co-Based Catalyst
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Carbon Number Dependence of Reaction Mechanism and Kinetics in CO Hydrogenation on a Co-Based Catalyst

机译：钴基催化剂上加氢反应机理和动力学的碳数依赖性

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摘要

A detailed mapping of the kinetic parameters involved in the reaction network of CO hydrogenation on a Co-Re/CNT catalyst has been performed. Multicomponent steady-state isotopic transient kinetic analysis (SSITKA) has been used to deconvolute the rates of chain growth and termination to olefins and paraffins with various carbon numbers into the concentration of the surface intermediates and their reactivity, expressed as their rate constants k(g), k(o), and k(p), respectively, at a molecular level. The site coverage of the different products (theta(Cn)) measured by the multicomponent analysis of their isotopic distribution allows the study of their effect on chain growth, as well as on olefin and paraffin formation. The insights into the reaction mechanism were gained from the kinetic dependence of different reaction steps on the hydrogen pressure. The results revealed a significant carbon number dependence of the mechanism for the chain growth and termination to paraffin and olefin reactions: an enol-like intermediate is dominating for the formation of C-3 hydrocarbons, while the alkenyl intermediate is dominating for the formation of C-4 hydrocarbons. Moreover, the SSITKA-assisted kinetic study provided the carbon number dependence of the rate constants of various reaction steps for the paraffin formation and chain growth, both decrease concurrently with increasing carbon number. However, the rate constant for the olefin formation is constant, regardless of the carbon number, suggesting the formation rate of olefins with different carbon number depends mainly on the concentration of the corresponding surface intermediates.
机译：已经完成了在Co-Re / CNT催化剂上进行CO加氢反应网络的动力学参数的详细映射。多组分稳态同位素瞬态动力学分析（SSITKA）已用于将链增长和各种碳原子数的烯烃和链烷烃的终止速率解卷积为表面中间体的浓度及其反应性，用速率常数k（g ），k（o）和k（p）分别处于分子水平。通过同位素分布的多组分分析测量的不同产物（θ（Cn））的位点覆盖范围允许研究它们对链增长以及对烯烃和石蜡形成的影响。从不同反应步骤对氢气压力的动力学依赖性中获得了对反应机理的见解。结果表明，链增长和终止至链烷烃和烯烃反应的机理对碳数具有显着依赖性：烯醇状中间体在C-3烃的形成中占主导地位，而烯基中间体在C-3烃的形成中占主导地位。 -4碳氢化合物。此外，SSITKA辅助的动力学研究提供了不同反应步骤的速率常数对石蜡形成和链增长的碳数依赖性，两者均随着碳数的增加而降低。然而，无论碳数如何，烯烃形成的速率常数都是恒定的，这表明具有不同碳数的烯烃的形成速率主要取决于相应的表面中间体的浓度。

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