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首页> 外文期刊>Catalysis science & technology >Discrimination of the mechanism of CH4 formation in Fischer-Tropsch synthesis on Co catalysts: a combined approach of DFT, kinetic isotope effects and kinetic analysis
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Discrimination of the mechanism of CH4 formation in Fischer-Tropsch synthesis on Co catalysts: a combined approach of DFT, kinetic isotope effects and kinetic analysis

机译：在Fischer-Tropsch合成中歧视CH4形成机制在CO催化剂上：DFT，动力学同位素效应和动力学分析的组合方法

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The mechanism of CH4 formation during Fischer-Tropsch synthesis on cobalt has been studied. DFT, kinetic isotope effect and kinetic analyses are combined to discriminate between the possible reaction routes of CH4 formation on Co catalysts. Nine direct reaction mechanisms were proposed from 21 elementary steps. They were first screened by DFT calculations in which the activation energies as well as the free energy profiles in each direct mechanism were compared, resulting in a reduction to six reaction mechanisms. Additional reduction was based on kinetic analysis where the reaction order was used as a descriptor. Subsequently, the kinetic isotope effect (KIE) values were calculated and compared to our previous SSITKA results. Finally, the dominating reaction route was suggested, which follows the initial elementary steps with H-assisted CO activation to form HCOH via HCO as an intermediate. It then proceeds through HCOH dissociation to CH followed by stepwise hydrogenation to CH4.
机译：已经研究了Fischer-Tropsch合成过程中CH4形成的机理。 DFT，动力学同位素效应和动力学分析被合并，以区分CO催化剂上CH4形成的可能反应途径。 从21个基本步骤提出了九种直接反应机制。 首先通过DFT计算对它们进行筛选，其中比较了每个直接机制中的激活能以及自由能谱，从而减少了六种反应机制。 额外的还原是基于动力学分析，其中反应顺序用作描述符。 随后，计算了动力学同位素效应（KIE）值，并将其与我们以前的SSITKA结果进行了比较。 最后，提出了主导的反应途径，该途径遵循HCO的初始基本步骤，并通过HCO激活HCO，作为中间体形成HCOH。 然后，它通过HCOH分离到CH，然后逐步氢化为CH4。

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