哌啶在MoP表面C—N键断裂反应实验设计

Design of Experiment on the C—N Bond Cleavage Mechanisms of Piperidine on MoP Surface

设计了哌啶在Mo P表面C—N键断裂反应机理实验,给出了哌啶在MoP(001)表面加氢脱氮反应中的C—N键断裂机理。哌啶在MoP(001)上存在4种稳定的吸附构型,均通过N—Mo键吸附在Mo原子顶位且吸附较弱,C—N键并未受到活化作用。哌啶E1消去过程(质子化+C—N键断裂)包含的反应能垒均比哌啶C—N键直接断裂能垒小很多,因此哌啶是通过E1消去反应而发生C—N键断裂的。该实验以超算中心为平台,使用Materials Studio软件开展密度泛函理论计算,可为材料计算类实验的开展提供思路和经验。

The experiment of'the C—N bond cleavage mechanisms of piperidine on MoP surface'is designed and studied,the C—N bond cleavage mechanisms of hydrodenitrogenation process on MoP(001)surface are presented.Piperidine has four types of adsorption configurations on MoP(001),which bind weakly at the atop Mo site through N—Mo bond.The C—N bond is not activated in these adsorption configurations.Since the activation energy barriers of E1 elimination reactions(protonation+C—N bond cleavage)are much lower than that of direct C—N bond cleavage,piperidine prefers E1 elimination rather than direct C—N bond cleavage,which provides theoretical guidance to some extent for the design of related catalysts.In this experiment,the computing hardware is supported by the supercomputing center,and the density functional calculations are performed by using the Materials Studio software.Through this article,we hope to provide ideas and experience for conducting experimental courses of computational materials science.