環己烷（C6H12）通常用作替代真實環烷烴的燃料，用於研究航空燃料的動力學，並從氧化角度進行了研究。為了了解涉及環己烷氧化反應生成化學物質的目標，本研究從零維點火延遲時間（T = 650-1812 K，P = 8-50 atm，ϕ = 0.5-2.0）方面檢驗了現有機制的預測準確性、一維火焰速度（Tu = 298-473 K，P = 1-10 atm，ϕ = 0.5-1.7）和零維噴射攪拌反應器中的物種分佈（T = 500-1100 K，P = 1-10 atm，ϕ = 0.5 -2.0）。在測試的現有動力學機制中，具有138種化學物質和584個反應的機制被認為是預測點火延遲時間和噴射攪拌反應器的最準確的數據庫。本研究進一步添加了缺失的物種和缺失的傳輸數據，以便全面預測零維非預混同流火焰中的不飽和正鏈烴和多環芳香烴（PAH）。透過更新速率常數以改善一維預混合層流管狀火焰中火焰速度和物種分佈的預測精度。透過去除機制中的其他燃料成分，可生成最小的骨架環己烷-多環芳香烴機制，具有128種化學物質和710個反應。研究的化學式包括萘（C10H8），苊烯（C12H8），芴（C13H10），菲（C14H10），蒽（C14H10），熒蒽（C16H10）和芘（C16H10），已被美國環境保護局（USEPA）分類為致癌和致突變的化合物，對人體健康具有影響。首次，使用反應路徑分析解釋了在甲烷添加環己烷的並流非預混火焰中，透過光電離飛行時間質譜儀量測到的15種碳氫化合物的摩爾分率。並結合了128種化學物質的精簡骨架機制的二維計算流體力學模型進行了計算驗證。

Cyclohexane, commonly used as a surrogate fuel to study the kinetics of aviation fuel, is investigated in terms of oxidation. Toward the goals of understanding the chemistry involving in oxidation of cyclohexane, the study examines the prediction accuracy of the existing mechanism in terms of ignition delay times (T = 650-1812 K, P = 8-50 atm, ϕ = 0.5-2.0), flame speeds (Tu = 298-473 K, P = 1-10 atm, ϕ = 0.5-1.7) and species profiles in a jet stirred reactor (T = 500-1100 K, P = 1-10 atm, ϕ = 0.5-2.0). Among the existing kinetic mechanisms tested, a mechanism with 138 species and 584 reactions is identified to be the most accurate database to predict ignition delay times and jet stirred reactors. The present study further adds missing species and missing transport data in order to comprehensively predicting unsaturated normal chain hydrocarbons and polycyclic aromatic hydrocarbons (PAHs) in a non-premixed co-flow flame. The rate constants are updated for refining the prediction accuracy of flame speed and the species profiles in premixed laminar tubular flame. By removing the multifuel components in the mechanism, a minimized skeletal cyclohexane-PAH mechanism is generated with 128 species and 710 reactions. The investigated chemical formulas include naphthalene (C10H8), acenaphthylene (C12H8), fluorene (C13H10), phenanthrene (C14H10), anthracene (C14H10), fluoranthene (C16H10) and pyrene (C16H10), which are up to 4 rings and have been classified by the United States Environmental Protection Agency (USEPA) as the carcinogenic and mutagenic compounds to human health. For the first time, previously measured mole fractions of 15 hydrocarbons in the co-flow flame by photoionization time-of-flight mass spectrometer are computationally interpreted by the present 2-D CFD model coupled with the 128-species mechanism.

Table of Contents
中文摘要 i
Abstract ii
Table of Contents iii
List of Table v
List of Figure vii
Nomenclature xii
Chpater 1 Introduction 1
1.1 Background 1
1.1.1 Oxidation formation of cyclohexane 1
1.1.2 PAH and soot formation 2
1.2 Literature review 4
1.2.1 Experimental study of cyclohexane 4
1.2.2 Modeling study of cyclohexane 8
1.3 Objective 12
Chpater 2 Methodology 13
2.1 Mechanism construction 13
2.1.1 Mechanism construction for cyclohexane 13
2.2 0-D ignition delay time 18
2.3 0-D jet-stirred reactor 19
2.4 1-D Flame speed 20
2.5 1-D premixed laminar tubular flame 23
2.6 Mechanism reduction 25
2.7 2-D co-flow flame 27
2.8 Preliminary investigations 33
Chpater 3 Results and discussion 45
3.1 Oxidation of cyclohexane 45
3.1.1 Mechanism construction and reduction 45
3.1.2 0-D ignition delay time 47
3.1.3 0-D jet-stirred reactor 52
3.1.4 1-D Flame speed 60
3.1.5 1-D premixed laminar tubular flame 63
3.1.6 2-D co-flow flame 66
Chpater 4 Conclusion 80
References 82
Appendix 86
Cyclohexane mechanism 86
Cyclohexane thermal data 95
Cyclohexane transport data 103

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