Optimal Catalyst Curves: Connecting Density Functional Theory Calculations with Industrial Reactor Design and Catalyst Selection
Optimal Catalyst Curves: Connecting Density Functional Theory Calculations with Industrial Reactor Design and Catalyst Selection
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最佳催化剂曲线：将密度泛函理论计算与工业反应器设计和催化剂选择联系起来
DOI：
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发表时间：
2002
期刊：
影响因子：
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通讯作者：
J. Nørskov
中科院分区：
文献类型：
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作者：
C. Jacobsen;S. Dahl;A. Boisen;B. Clausen;H. Topsøe;Á. Logadóttir;J. Nørskov
氨合成催化剂在实验中发现了一种火山型关系。我们表明，通过结合密度泛函理论计算与微观动力学模型的火山曲线的最大值的位置是敏感的反应条件。催化氨合成活性，在第一近似下，仅是氮与催化剂的结合能的函数。因此，可以评估在给定的反应条件下哪种氮结合能是最佳的。这导致了最佳催化剂曲线的概念，其示出了在不同温度、压力和合成气组成下的最佳催化剂的氮结合能。利用这一概念以及制备具有所需结合能的催化剂的能力，可以优化氨工艺。这样，第一次建立了气体-表面相互作用的第一性原理量子力学计算、反应器设计和催化剂选择之间的联系。
Abstract For ammonia synthesis catalysts a volcano-type relationship has been found experimentally. We demonstrate that by combining density functional theory calculations with a microkinetic model the position of the maximum of the volcano curve is sensitive to the reaction conditions. The catalytic ammonia synthesis activity, to a first approximation, is a function only of the binding energy of nitrogen to the catalyst. Therefore, it is possible to evaluate which nitrogen binding energy is optimal under given reaction conditions. This leads to the concept of optimal catalyst curves, which illustrate the nitrogen binding energies of the optimal catalysts at different temperatures, pressures, and synthesis gas compositions. Using this concept together with the ability to prepare catalysts with desired binding energies it is possible to optimize the ammonia process. In this way a link between first-principle quantum mechanical calculations of gas–surface interactions, reactor design, and catalyst selection has been established for the first time.