Resolving discrepancies in detailed kinetic models of combustion via automated transition state theory calculations

通过自动过渡态理论计算解决详细燃烧动力学模型中的差异

• 批准号: 1605568
• 负责人: Richard West
• 金额: $ 26万
• 依托单位: Northeastern University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2016
• 资助国家: 美国
• 起止时间: 2016-07-01 至 2020-04-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1605568&HistoricalAwards=false
• 关键词: Resolving; discrepancies; detailed; kinetic; models

1605568 WestIn order to develop cleaner and more efficient engines, and to make better use of both petroleum-derived and alternative fuels, engineers need a better understanding of combustion. Computer models that can accurately predict how different fuels burn in different conditions will help us develop new engines and new fuels. The goal of this research is predictive, detailed kinetic modeling of combustion, in which many thousands of relevant chemical reactions are calculated accurately. As a step towards this goal, the research will detect and correct major discrepancies in the reaction rates currently used in detailed kinetic models, and in so doing create a database of reaction transition states, as well as algorithms to predict them. The proposed work will use several novel techniques to identify and correct mistakes, uncertainties, and approximations currently hidden throughout detailed kinetic models of combustion. The project will remove the human bottle-neck in performing quantum mechanical calculations of chemical kinetics, enabling effective use of High Performance Computing for accurate calculation of reaction rate expressions in the future. This high-throughput calculation of reaction kinetics has been identified as a "basic research need for clean and efficient combustion of 21st century transportation fuels", and by the Combustion Energy Frontier Research Center as an "important grand challenge".This three year project proposes to: (1) automate the performance of quantum mechanics (QM) based Transition State Theory (TST) calculations for combustion-relevant reactions in the open-source, kinetic model building software Reaction Mechanism Generator (RMG); (2) use a newly developed kinetic model importer tool to identify every elementary reaction published in recent combustion models; (3) use the automated methods from step one to calculate the rates of reactions from step two, creating a public database of reactions, rates from the literature, rates calculated by TST, QM calculation results, and transition state geometries; and (4) identify discrepancies between reaction rates in published models and those calculated via TST, and quantify the effect these discrepancies have on the model predictions. Additionally, we will develop a related suite of Python-based teaching materials suitable for undergraduate chemical engineering curriculum, to introduce combustion science to a wider audience. A PhD student and several undergraduate students will gain valuable research experience and training whilst working on this project.

1605568 Westin下令开发清洁剂，更高效的发动机，并更好地利用石油来源和替代燃料，工程师需要更好地了解燃烧。可以准确预测不同燃料在不同条件下如何燃烧的计算机模型将帮助我们开发新的发动机和新燃料。这项研究的目的是燃烧的​​预测性动力学建模，其中准确计算了数千种相关的化学反应。作为朝着这一目标迈出的一步，研究将检测并纠正当前在详细动力学模型中使用的反应率的主要差异，并因此创建一个反应过渡状态的数据库以及预测它们的算法。拟议的工作将使用几种新颖的技术来识别和纠正当前隐藏在详细的燃烧动力学模型中的错误，不确定性和近似值。该项目将在进行化学动力学的量子机械计算时删除人瓶颈，从而有效利用高性能计算以准确计算未来的反应速率表达式。 This high-throughput calculation of reaction kinetics has been identified as a "basic research need for clean and efficient combustion of 21st century transportation fuels", and by the Combustion Energy Frontier Research Center as an "important grand challenge".This three year project proposes to: (1) automate the performance of quantum mechanics (QM) based Transition State Theory (TST) calculations for combustion-relevant reactions in the open-source,动力学模型构建软件反应机理生成器（RMG）； （2）使用新开发的动力学模型进口工具来识别最近燃烧模型中发表的每个基本反应； （3）使用第一步中的自动化方法来计算第二步的反应速率，创建一个公共反应数据库，文献速率，TST计算的速率，QM计算结果以及过渡状态几何； （4）确定已发布模型中反应速率与通过TST计算的反应速率之间的差异，并量化这些差异对模型预测的影响。此外，我们将开发一套相关的基于Python的教材，适合本科化学工程课程，以向更广泛的受众介绍燃烧科学。一名博士生和几位本科生将在该项目工作时获得宝贵的研究经验和培训。

项目成果

The impact of roaming radicals on the combustion properties of transportation fuels

漫游自由基对运输燃料燃烧性能的影响

• DOI: 10.1016/j.combustflame.2018.05.020
• 发表时间: 2018
• 期刊: Combustion and Flame
• 影响因子: 4.4
• 作者: West, Richard H.;Goldsmith, C. Franklin
• 通讯作者: Goldsmith, C. Franklin