Experimental investigation and kinetic modeling of n-propylbenzene oxidation under high-pressure conditions

IF 4.1 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science Pub Date : 2025-04-11 DOI:10.1016/j.ces.2025.121653

Xu-Peng Yu , Du Wang , Xu Zhang , Xiang Gao , Ahmed E. Mansy , Jin-Hu Yang , Zhen-Yu Tian

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Abstract

In this study, oxidation experiments of n-propylbenzene (NPB) were conducted at 24 atm, with equivalence ratios (Φ = 0.5, 1.0, and 2.0), and temperatures ranging from 640-820 K. A total of 17 products and intermediates were qualitatively and quantitatively detected using gas chromatography (GC) and gas chromatography-mass spectrometry (GC–MS). The most important rate coefficients, H-abstraction reactions by OH at the α, β, and γ carbon sites of the side chain, were theoretically calculated at G4//wb97xd/6-311 + g(d,p) level. A comprehensive oxidation model of NPB, comprising 285 species and 1953 elementary reactions was constructed to understand the high-pressure oxidation. The model was extensively validated across a pressure range of 1–50 atm using oxidation data from JSR reactor, mole fraction data from shock tube, ignition delay time, and laminar flame speed. According to the selectivity of products analysis, high pressure promotes the complete progression of the reaction and reduces the formation of PAHs.

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高压条件下正丙苯氧化的实验研究与动力学建模

本研究在 24 个大气压、等效比（Φ = 0.5、1.0 和 2.0）和 640-820 K 的温度范围内进行了正丙基苯（NPB）的氧化实验。利用气相色谱（GC）和气相色谱-质谱法（GC-MS）对总共 17 种产物和中间产物进行了定性和定量检测。在 G4//wb97xd/6-311+g(d,p)水平上对侧链 α、β 和 γ 碳位点上的羟基萃取反应中最重要的速率系数进行了理论计算。为了理解 NPB 的高压氧化过程，我们构建了一个包含 285 个物种和 1953 个基本反应的 NPB 综合氧化模型。利用 JSR 反应器的氧化数据、冲击管的分子分数数据、点火延迟时间和层流火焰速度，在 1-50 atm 的压力范围内对该模型进行了广泛验证。根据产物的选择性分析，高压促进了反应的完全进行，并减少了多环芳烃的生成。

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来源期刊

Chemical Engineering Science 工程技术-工程：化工

CiteScore

7.50

自引率

8.50%

发文量

1025

审稿时长

50 days

期刊介绍： Chemical engineering enables the transformation of natural resources and energy into useful products for society. It draws on and applies natural sciences, mathematics and economics, and has developed fundamental engineering science that underpins the discipline. Chemical Engineering Science (CES) has been publishing papers on the fundamentals of chemical engineering since 1951. CES is the platform where the most significant advances in the discipline have ever since been published. Chemical Engineering Science has accompanied and sustained chemical engineering through its development into the vibrant and broad scientific discipline it is today.