Development of a methodology for determining reaction pathways and rate constants of complex combustion networks

开发确定复杂燃烧网络的反应路径和速率常数的方法

• 批准号: 322657802
• 负责人: Professor Dr. Kai Leonhard
• 金额: --
• 依托单位: Lehrstuhl für Technische Thermodynamik (LTT)
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2016
• 资助国家: 德国
• 起止时间: 2015-12-31 至 2020-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/322657802?language=en
• 关键词: Development; methodology; determining; reaction; pathways

In many chemical and combustion engineering applications, chemical reaction mechanisms are required to model and optimize processes and devices accurately. Due to the large number of reactions and species, often the determination of rate coefficients of all elementary reactions is not possible from experimentally accessible data. Therefore, experiments have been augmented by ab initio calculations in the last years. Such calculations, however, require much chemical intuition, large amounts of human and computer time, and still their accuracy sometimes suffers from the simplifications made in the models used. In this work, we suggest to overcome these issues by performing molecular dynamics simulations with a reactive force field to automatically identify reaction paths and transition states. The latter ones will be refined in an automated procedure by quantum mechanics and used to compute reaction rates. Molecular simulations can also be used to relax some of the assumptions made in the transition state theory models usually used. Therefore, we expect to develop a methodology that will allow the determination of reaction models more efficiently and with higher accuracy than it is presently possible. This methodology will be used to investigate the ignition properties and the formation of pollutants of novel biofuels.

在许多化学和燃烧工程应用中，需要化学反应机制来精确地建模和优化过程和设备。由于大量的反应和物种，通常不可能从实验获得的数据确定所有基元反应的速率系数。因此，在过去的几年里，实验已经通过从头计算得到了加强。然而，这种计算需要大量的化学直觉、大量的人力和计算机时间，而且它们的准确性有时仍会受到所使用模型的简化的影响。在这项工作中，我们建议通过进行分子动力学模拟与反应力场自动识别反应路径和过渡态来克服这些问题。后者将在量子力学的自动程序中进行改进，并用于计算反应速率。分子模拟也可以用来放松通常使用的过渡态理论模型中的一些假设。因此，我们希望开发一种方法，使反应模型的确定更有效，更高的精度比目前可能的。该方法将用于研究新型生物燃料的点火特性和污染物的形成。