Development of a detailed kinetic model for high-pressure ethanol oxidation in gas phase and supercritical water

IF 3.4 3区工程技术 Q2 CHEMISTRY, PHYSICAL

Journal of Supercritical Fluids Pub Date : 2023-10-01 DOI:10.1016/j.supflu.2023.106025

Guoxing Li , Hao Chen , Yipu Zhang , Hongming Xu , Mingbo Niu , Chuang Yang

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Abstract

The present study aims to develop a detailed chemical kinetic model for high-pressure ethanol oxidation in the gas phase and supercritical water (SCW). Kinetic parameters for key elementary reactions involving HO₂ and CH₃OO radicals were updated, deriving from a careful analysis of ignition delay data or analogy. The model performance is validated comprehensively by comparison to a wide variety of recent experimental data from both gas-phase and SCW conditions. The model predicted ignition delay times and speciation measurements (15–60 bar) in the gas phase fairly well. Additionally, the model showed satisfactory performance in reproducing the species concentration profiles at SCW conditions. A comparative kinetic analysis was further conducted to investigate the characteristic differences and similarities of ethanol oxidation at the two conditions. The results indicated SCW lowered the onset temperature for ethanol ignition and facilitated the ethanol oxidation rate, but did not introduce additional oxidation pathways.

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建立了气相和超临界水中高压乙醇氧化动力学模型

本研究旨在建立一个详细的气相和超临界水（SCW）中高压乙醇氧化的化学动力学模型。通过对点火延迟数据或类比的仔细分析，更新了涉及HO2和CH3OO自由基的关键基本反应的动力学参数。通过与气相和SCW条件下的各种最新实验数据进行比较，全面验证了模型性能。该模型很好地预测了气相中的点火延迟时间和形态测量（15–60巴）。此外，该模型在SCW条件下再现物种浓度分布方面表现出令人满意的性能。进一步进行了比较动力学分析，以研究在两种条件下乙醇氧化的特征差异和相似性。结果表明，SCW降低了乙醇着火的起始温度，促进了乙醇的氧化速率，但没有引入额外的氧化途径。

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

Journal of Supercritical Fluids 工程技术-工程：化工

CiteScore

7.60

自引率

10.30%

发文量

236

审稿时长

56 days

期刊介绍： The Journal of Supercritical Fluids is an international journal devoted to the fundamental and applied aspects of supercritical fluids and processes. Its aim is to provide a focused platform for academic and industrial researchers to report their findings and to have ready access to the advances in this rapidly growing field. Its coverage is multidisciplinary and includes both basic and applied topics. Thermodynamics and phase equilibria, reaction kinetics and rate processes, thermal and transport properties, and all topics related to processing such as separations (extraction, fractionation, purification, chromatography) nucleation and impregnation are within the scope. Accounts of specific engineering applications such as those encountered in food, fuel, natural products, minerals, pharmaceuticals and polymer industries are included. Topics related to high pressure equipment design, analytical techniques, sensors, and process control methodologies are also within the scope of the journal.