Liu Runcong
Center of Materials Science and Optoelectronics Engineering, College of Materials Science and Opto-Electronic Technology, University of Chinese Academy of Sciences, Beijing 100049, China.
ACS Omega. 2021 Oct 29;6(44):29432-29448. doi: 10.1021/acsomega.1c03292. eCollection 2021 Nov 9.
In most studies, the microkinetics for multistep reactions are numerically solved due to their complexity; the obtained numerical results are only valid under given reaction conditions at a static point. In this work, the microkinetics of heterogeneously catalyzed hydrogenation reactions are analytically solved as a function of three coupled physical parameters, which are energy, reaction rate, and coverage. The results correlate the surface reactions and the gaseous-phased reactant/product by energy and thus provide a dynamic view over the whole reaction process rather than at a static point. The analytical expressions are given for a simple hydrogenation reaction and three more complicated hypothetical hydrogenation reactions with side products, side reaction paths, or even multiple active sites. Compared with the numerical solution, the analytical solution is valid under all reaction conditions in practice and can provide more guidance to optimize the overall outcome or catalyst development.
在大多数研究中，由于多步反应的微观动力学较为复杂，通常采用数值求解的方法；所得到的数值结果仅在给定反应条件下的静态点有效。在本工作中，非均相催化氢化反应的微观动力学作为能量、反应速率和覆盖率这三个耦合物理参数的函数进行了解析求解。结果通过能量将表面反应与气相反应物/产物关联起来，从而提供了整个反应过程的动态视图，而非仅仅是静态点的情况。文中给出了一个简单氢化反应以及另外三个更复杂的假设氢化反应（有副产物、副反应路径甚至多个活性位点）的解析表达式。与数值解相比，解析解在实际的所有反应条件下均有效，并且能够为优化整体结果或催化剂开发提供更多指导。
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