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准确对过程和设备进行建模。由于反应和物种数量众多，通常无法从实验可访问的数据中确定所有基本反应的速率系数。因此，在过去几年中，从头算的计算已经增加了实验。但是，这样的计算需要大量的化学直觉，大量的人力和计算机时间，并且其准确性有时会遭受模型中所做的简化。在这项工作中，我们建议通过使用反应力场进行分子动力学模拟来克服这些问题，以自动识别反应路径和过渡态。后者将通过量子力学以自动化程序进行完善，并用于计算反应速率。分子模拟也可以用于放松通常使用的过渡状态理论模型中的某些假设。因此，我们期望开发一种方法，该方法将使反应模型更有效，准确性比目前可能更高。该方法将用于研究新型生物燃料的污染物的点火特性和形成。