Exploring the interaction kinetics of butene isomers and NO$_{x}$ at low temperatures and diluted conditions
Exploring the interaction kinetics of butene isomers and NO$_{x}$ at low temperatures and diluted conditions
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DOI：
10.1016/j.combustflame.2021.111557
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发表时间：
2021-11
影响因子：
4.4
通讯作者：
Sabrina Gossler;L. Ruwe;Wenhao Yuan;Jiuzhong Yang;Xiamin Chen;Steffen Schmitt;L. Maier;K. Kohse-Höing
中科院分区：
文献类型：
--
作者：
Sabrina Gossler;L. Ruwe;Wenhao Yuan;Jiuzhong Yang;Xiamin Chen;Steffen Schmitt;L. Maier;K. Kohse-Höing
实验和数值研究了1-丁烯和二丁烯的氧化与不添加1000 ppm NO主要是在富燃料（φ = 2.0）的条件下，在高稀释（96% Ar），在流动反应器在大气压下运行，低温范围约600-1200 K。采用同步加速器真空紫外光电离质谱法（SVUV-PIMS）对多种中间物质进行了检测和定量。在文献资料和本工作的基础上，建立了由682种物质中3996个反应组成的初阶反应机理，描述了丁烯同分异构体与氧、氮组分的反应及其相互作用动力学。将模型预测结果与实验结果进行比较，以深入了解不添加NO和添加NO的低温和高温燃料消耗以及各自的相互作用化学。这项研究首先为这两种丁烯异构体在与发动机废气有关的条件下提供了一套一致的温度依赖浓度曲线。其次，观察到的氧化动力学随着NO的加入而显著改变。具体来说，NO促进了燃油消耗，并引入了具有负温度系数（NTC）区域的对戊丁烯低温行为。该模型与主要产物和中间产物的实验结果吻合较好，能够解释NO对自由基池的贡献所产生的促进作用。此外，通过反应流分析和灵敏度分析，该模型还可以描述由于链扩展和链终止反应的竞争，所观察到的丁烯/NO混合物的NTC区。
The oxidation of 1-butene andi-butene with and without addition of 1000 ppm NO was experimentally and numerically studied primarily at fuel-rich (ϕ= 2.0) conditions under high dilution (96% Ar) in a flow reactor operated at atmospheric pressure in the low temperature range of approximately 600-1200 K. Numerous intermediate species were detected and quantified using synchrotron vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS). An elementary-step reaction mechanism consisting of 3996 reactions among 682 species, based on literature and this work, was established to describe the reactions and interaction kinetics of the butene isomers with oxygen and nitrogenous components. Model predictions were compared with the experimental results to gain insight into the low- and high-temperature fuel consumption without and with NO addition and thus the respective interaction chemistry. This investigation firstly contributes a consistent set of temperature-dependent concentration profiles for these two butene isomers under conditions relevant for engine exhaust gases. Secondly, the observed oxidation kinetics is significantly altered with the addition of NO. Specifically, NO promotes fuel consumption and introduces fori-butene a low-temperature behavior featuring a negative temperature coefficient (NTC) region. The present model shows reasonable agreement with the experimental results for major products and intermediate species, and it is capable to explain the promoting effect of NO that is initiated by its contribution to the radical pool. Further, it can describe the observed NTC region for thei-butene/NO mixture as a result of the competition of chain propagation and chain terminating reactions that were identified by reaction flow and sensitivity analyses.