Developing chemical kinetic models for thermochemical applications.

IF 13.1 1区 生物学 Q1 BIOCHEMICAL RESEARCH METHODS
Marco Mehl, Matteo Pelucchi, Luna Pratali Maffei, Alessandro Stagni, Alberto Cuoci, Alessio Frassoldati, Eliseo Ranzi, Tiziano Faravelli
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引用次数: 0

Abstract

A general procedure for the development of chemical kinetic models relevant to thermochemical applications (pyrolysis, gasification and combustion) is described. Here we present techniques that aim at producing models that are modular in structure, thoroughly validated, and applicable to a wide variety of conditions (generality), while balancing accuracy and computational burden. Starting from a core mechanism describing the pyrolysis and oxidation of light species, heavier compounds are added to the model in a hierarchical fashion, starting from archetypal species of each class of compounds. Using analogy rules derived from the archetypal species, a list of reactions and reaction rate parameters are compiled for molecules belonging to the classes of interest, obtaining detailed or semidetailed reaction mechanisms. The model is then validated using data available from the literature and/or novel experiments performed ad hoc. Depending on the applications of interest and on the size of the model, a mechanism reduction can be performed using a combination of lumping techniques and flux or sensitivity analyses. These procedures, although partially automated, still require some level of expert knowledge. The development of reaction rate rules and the identification of reaction pathways require indeed critical analysis and are most effective when the operator has previous experience in the field. A rigorously built mechanism, obeying the general principles presented here, provides high predictivity and permits extrapolating fuel behavior with greater confidence outside the range of validation conditions compared with models assembled from nonconsistently sourced submechanism from the literature, or based on limited datasets and empirical information.

开发热化学应用的化学动力学模型。
描述了开发与热化学应用(热解、气化和燃烧)相关的化学动力学模型的一般程序。在这里,我们提出的技术旨在产生模块化结构的模型,经过彻底验证,并适用于各种条件(通用性),同时平衡准确性和计算负担。从描述轻组分热解和氧化的核心机制开始,从每一类化合物的原型组分开始,以分层方式将较重的化合物添加到模型中。利用源自原型物种的类比规则,编制了属于感兴趣类别的分子的反应和反应速率参数列表,获得了详细或半详细的反应机理。然后使用从文献中获得的数据和/或临时进行的新实验来验证该模型。根据感兴趣的应用和模型的大小,可以使用集总技术和通量或灵敏度分析相结合的方法进行机制约简。这些程序虽然部分自动化,但仍然需要一定程度的专业知识。反应速率规则的制定和反应路径的确定确实需要严格的分析,并且当操作人员具有该领域的经验时最有效。与从文献中不一致来源的子机制或基于有限数据集和经验信息组装的模型相比,遵循本文提出的一般原则的严格构建的机制提供了高预测性,并允许在验证条件范围之外更有信心地推断燃料行为。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Nature Protocols
Nature Protocols 生物-生化研究方法
CiteScore
29.10
自引率
0.70%
发文量
128
审稿时长
4 months
期刊介绍: Nature Protocols focuses on publishing protocols used to address significant biological and biomedical science research questions, including methods grounded in physics and chemistry with practical applications to biological problems. The journal caters to a primary audience of research scientists and, as such, exclusively publishes protocols with research applications. Protocols primarily aimed at influencing patient management and treatment decisions are not featured. The specific techniques covered encompass a wide range, including but not limited to: Biochemistry, Cell biology, Cell culture, Chemical modification, Computational biology, Developmental biology, Epigenomics, Genetic analysis, Genetic modification, Genomics, Imaging, Immunology, Isolation, purification, and separation, Lipidomics, Metabolomics, Microbiology, Model organisms, Nanotechnology, Neuroscience, Nucleic-acid-based molecular biology, Pharmacology, Plant biology, Protein analysis, Proteomics, Spectroscopy, Structural biology, Synthetic chemistry, Tissue culture, Toxicology, and Virology.
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