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Water gas shift reaction kinetics in Fischer-Tropsch synthesis over an industrial Fe-Mn catalyst

机译：工业Fe-Mn催化剂在费托合成中的水煤气变换反应动力学

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摘要

The kinetics of water gas shift (WGS) reaction over an Fe-Mn catalyst under Fischer-Tropsch synthesis (FTS) reaction conditions is studied in a spinning basket reactor. Experimental conditions are varied as follows: temperature of 533-573 K, reactor pressure of 10.0-26.5 bar, H_2/CO feed ratio of 0.66-2.0 and space velocity of 0.66-2.65 X 10~(-3) Nm~3 kg~(-1) s~(-1). By separately fitting WGS kinetics parameters with experimental data, which is possible in the spinning basket reactor with neglecting concentration and temperature gradients, different kinetics models of WGS are derived and discriminated on the basis of four sets of WGS elementary reactions. Kinetics experimental results show that the WGS reaction under FTS reaction conditions is far from equilibrium. Two types of WGS mechanisms are investigated. One is the formate mechanism, and the other is the direct oxidation mechanism. It is found that the formate mechanism is better in fitting experimental data than the direct oxidation mechanism over the Fe-Mn catalyst under the FTS reaction conditions. The optimized kinetics model with formate intermediate dissociation as the rate-determining step (RDS) can fit the WGS experimental results well. The simplified WGS kinetics model can easily be used for industrial modeling applications.
机译：在旋转篮式反应器中研究了费-托合成（FTS）反应条件下Fe-Mn催化剂上水煤气变换（WGS）反应的动力学。实验条件变化如下：温度为533-573 K，反应器压力为10.0-26.5 bar，H_2 / CO进料比为0.66-2.0，空速为0.66-2.65 X 10〜（-3）Nm〜3 kg〜 （-1）秒〜（-1）。通过将WGS动力学参数分别与实验数据拟合，而这在纺丝篮式反应器中可以忽略浓度和温度梯度，因此可以基于四组WGS基本反应推导和区分不同的WGS动力学模型。动力学实验结果表明，FTS反应条件下的WGS反应远未达到平衡。研究了两种类型的WGS机制。一种是甲酸盐机制，另一种是直接氧化机制。结果发现，在FTS反应条件下，甲酸机理优于对Fe-Mn催化剂的直接氧化机理。以甲酸酯中间体离解为速率确定步骤（RDS）的优化动力学模型可以很好地拟合WGS实验结果。简化的WGS动力学模型可以轻松地用于工业建模应用。

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