Multi-Component Reactive Pressure-dependent Chemistry Verified by Multi-Scale Uncertainty Quantification

新兴的内燃机技术显示出改善燃料经济性和减少环境污染的前景。然而，工程师面临着设计挑战，因为这些改进的发动机需要前所未有的精确控制燃料燃烧化学。优化设计现在需要燃烧化学的科学描述是前所未有的精确。这对于使用计算机模型的工程师来说尤其如此。为了满足这些需求，该项目的目标是创建和验证预测燃烧化学模型。这个项目将在分子水平上创建燃烧化学的描述，然后验证这些描述对燃烧测量。这项研究中的基本化学行为特征也将导致对行星大气的更好理解。最后，这个项目将把研究发现带到课堂上，培训研究生掌握最先进的计算机建模，并在学校参观和实验室图尔斯中与当地K-12学生分享科学思维过程。拟议研究的技术目标是创建一个多尺度，H2/CO/CH 2 O燃烧的不确定性量化模型，与第一性原理和燃烧实验相一致。一个主要的焦点是建立的现象学反应和速率定律的类型的高活性发动机环境，特别是对于非热动力学序列，具有复杂的依赖于温度，压力和混合物的组成。PI建议：1）对重要的非热动力学序列进行最先进的第一原理计算; 2）构建多尺度燃烧模型，直接将可从第一原理计算的分子行为与可在燃烧实验中测量的宏观行为联系起来; 3）测试模型与第一原理和燃烧实验的一致性，以通过逆不确定性量化来验证模型。到项目结束时，建立的反应类型和速率定律将作为燃烧和大气中其他反应的原型，产生的高精度模型将用于其他科学和工程应用。

Emerging combustion engine technologies show promise for improved fuel economy and reduced environmental pollution. However, engineers face design challenges because these improved engines require unprecedentedly precise control of fuel combustion chemistry. Optimal design now requires scientific descriptions of combustion chemistry to be unprecedentedly precise. This is especially true for engineers using computer models. To serve these needs, the project goal is to create and validate predictive combustion chemistry models. This project will create descriptions of combustion chemistry at the molecular level and then validate these descriptions against combustion measurements. The fundamental chemical behavior characterized in this research will also lead to a greater understanding of planetary atmospheres. Finally, this project will bring research discoveries to students in the classroom, train graduate students in state-of-the-art computer modeling, and share the scientific thought process with local K-12 students in school visits and lab tours.The technical objective of the proposed research is to create a multi-scale, uncertainty-quantified model of H2/CO/CH2O combustion that is consistent with both first principles and combustion experiments. A primary focus is establishing the types of phenomenological reactions and rate laws of highly reactive engine environments, especially for non-thermal kinetic sequences that have complex dependences on temperature, pressure, and mixture composition. The PI proposes to 1) perform state-of-the-art first principles calculations for important non-thermal kinetic sequences; 2) construct a multi-scale combustion model that directly bridges molecular behavior, calculable from first principles, to macroscopic behavior, measurable in combustion experiments; and 3) test model consistency with both first principles and combustion experiments to validate the model via inverse uncertainty quantification. By the project end, the established reaction types and rate laws will serve as prototypes for other reactions in combustion and atmospheres, and the produced high-accuracy model will be ready to use in other scientific and engineering applications.