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Overcoming ammonia synthesis scaling relations with plasma-enabled catalysis
Nature Catalysis ( IF 37.8 ) Pub Date : 2018-04-02 , DOI: 10.1038/s41929-018-0045-1
Prateek Mehta , Patrick Barboun , Francisco A. Herrera , Jongsik Kim , Paul Rumbach , David B. Go , Jason C. Hicks , William F. Schneider

Correlations between the energies of elementary steps limit the rates of thermally catalysed reactions at surfaces. Here, we show how these limitations can be circumvented in ammonia synthesis by coupling catalysts to a non-thermal plasma. We postulate that plasma-induced vibrational excitations in N2 decrease dissociation barriers without influencing subsequent reaction steps. We develop a density-functional-theory-based microkinetic model to incorporate this effect, and parameterize the model using N2 vibrational excitations observed in a dielectric-barrier-discharge plasma. We predict plasma enhancement to be particularly great on metals that bind nitrogen too weakly to be active thermally. Ammonia synthesis rates observed in a dielectric-barrier-discharge plasma reactor are consistent with predicted enhancements and predicted changes in the optimal metal catalyst. The results provide guidance for optimizing catalysts for application with plasmas.



中文翻译:

用等离子体催化克服氨合成结垢关系

基本步骤的能量之间的相关性限制了表面热催化反应的速率。在这里,我们展示了如何通过将催化剂偶联至非热等离子体来避免氨合成中的这些局限性。我们假设在N 2中等离子体诱导的振动激发降低了解离势垒,而不会影响随后的反应步骤。我们开发了一种基于密度泛函理论的微动力学模型来吸收这种影响,并使用N 2对模型进行参数化在介电势垒放电等离子体中观察到振动激发。我们预测,对于与氮结合得太弱而无法热活化的金属,等离子体的增强作用尤其明显。在介电势垒放电等离子体反应器中观察到的氨合成速率与最佳金属催化剂中预期的增强和预测的变化相一致。结果为优化用于等离子体的催化剂提供了指导。

更新日期:2018-04-03
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